Condensed Matter Nuclear Science: Proceedings of the 12th International Conference on Cold Fusion, Yokohama, Japan 27 November-2 December 2005

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ondensed m after n uclear cience proceedings of the 12th international conference on cold fusion

Yokohama, Japan 27 November - 2 December 2005

Editors

Akito Takahashi Osaka University, Japan

Ken-ichiro Ota Yokohama National University, Japan

Yasuhiro Iwamura Mitsubishi Heavy Industries, Japan

\[p World Scientific NEW JERSEY • LONDON

• SINGAPORE

• BEIJING

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CHENNAI

Published by World Scientific Publishing Co. Pte. Ltd. 5 Toh Tuck Link, Singapore 596224 USA office: 27 Warren Street, Suite 401-402, Hackensack, NJ 07601 UK office: 57 Shelton Street, Covent Garden, London WC2H 9HE

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CONDENSED MATTER NUCLEAR SCIENCE Proceedings of the Twelveth International Conference on Cold Fusion Copyright © 2006 by World Scientific Publishing Co. Pte. Ltd. All rights reserved. This book, or parts thereof, may not be reproduced in any form or by any means, electronic or mechanical, including photocopying, recording or any information storage and retrieval system now known or to be invented, without written permission from the Publisher.

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PREFACE The study of Condensed Matter Nuclear Science (CMNS) has continued to advance through 11 past conferences (ICCF1 at Utah, USA in 1989 to ICCF11 at Marseilles, France in 2004) and many new compelling scientific findings are becoming known. The historical 1989 claim of "cold fusion" had renewed hope of a portable clean nuclear reactor. The subsequent great wave of denial and hostility forced the claim and further research efforts out of mainstream science. Nevertheless, due to misconceptions and misinformation, very few people know that several hundred researchers from around the world have continued this research during the past 16 years. The efforts by this faint stream of research have now revealed that there exist new kinds of nuclear effects directly related to the nature of condensed matter. The nuclear effects in condensed matter are much more than real "cold fusion"; they include important nuclear effects such as transmutations and resulting release of energy as significant heat with minimal and safe radiation. Low levels of radiation are found in at least some reactions, but are usually absorbed within the cell itself so the system is categorically safe. Through discussions at international conferences (ICCF1-ICCF11), a majority of researchers agreed that the name "cold fusion" was misleading. A new name, closer to the exact phenomenon, Condensed Matter Nuclear Science, is most appropriate. This emerging field, CMNS, treats nuclear effects in and/or on condensed matter, targeting its application for portable clean nuclear sources. This is an interand multi-disciplinary academic field, including nuclear physics, condensed matter physics, surface physics, and chemistry and electrochemistry. CMNS applications involve many other fields of science and technology (nuclear engineering, mechanical engineering, electrical engineering, laser science and engineering, material science, nano-technology, biotechnology, energy politics, etc. To promote the development of CMNS and establish the academic field of CMNS, the field needs highly efficient, cooperative efforts of researchers, and related people working in different fields. International linkage and collaborations are also needed. The full name of this conference is the 12th International Conference on Condensed Matter Nuclear Science. However, we decided to keep the acronym ICCF12 for the Conference, considering our original standpoint and tradition. The International Society for Condensed Matter Nuclear Science (ISCMNS) made a start in 2004 to promote the understanding, development and application of CMNS and has become a main supporting body of the ICCF series conferences till ICCF11. However, ICCF12 is sponsored by other societies like JCF (Japan-CF Research Society) and supported also by non-ISCMNS members. ICCF12 will provide an international scientific forum for direct interaction and stimulation among many scientists working in the CMNS field and participation and presentation of newcomers will be welcome. V

vi

The Conference site and date were: Shin-Yokohama Prince Hotel, Yokohamacity, Japan on 27 November-2 December 2005. The following topics were discussed in the conference: • • • • • • •

Excess Heat and Related Nuclear Products. Nuclear Processes and Transmutations. Materials and Condensed Matter Conditions. Analyses and Diagnoses Techniques. Innovative Approaches. Theories on Condensed Matter Nuclear Effects. Engineering, Industrial, Political, and Philosophical Issues.

For organizing and preparing ICCF12, the following members of LOC (Local Organizing Committee) and IAC (International Advisory Committee) have made contributions. Local Organizing Committee Akito Takahashi, Chairman, Osaka University, Japan. Ken-ichiro Ota, Co-chairman, Yokohama National University, Japan. Yasuhiro Iwamura, Co-chairman, Mitsubishi Heavy Industries, Japan. Shigenori Mitsushima, Secretary, Yokohama, National University, Japan. Shinya Narita, Secretary, Iwate University, Japan. Hiroshi Yamada, Iwate University, Japan. Tadahiko Mizuno, Hokkaido University, Japan. Akira Kitamura, Kobe University, Japan. Kazuaki Matsui, Institute of Applied Energy, Japan. Koichi Tomimura, The Thermal and Electric Energy Technology Foundation, Japan. International Advisory Committee Tullio Bressani, Department of di Fisica Sperimentale, Universita di Torino, Italy. Francesco Celani, INFN, Frascati, Italy. Antonella De Ninno, ENEA, Frascati, Italy. Peter Hagelstein, MIT, USA. Akito Takahashi, Osaka University, Japan. Ken-ichiro Ota, Department of Energy and Safety Engineering, Yokohama, National University, Japan. Jirohta Kasagi, Laboratory for Nuclear Science, Tohoku University, Japan. Yasuhiro Iwamura, Mitsubishi Heavy Industries, Japan. Xing Zhong Li, Tsinghua University, China. Andrei Lipson, Institute of Physical Chemistry, The Russian Academy of Sciences, Moscow, Russia.

vii

Michael McKubre, SRI International, USA. George Miley, Fusion Studies Laboratory, University of Illinois, USA. Nikolai Samsonenko, People Friendship University, Russia. Francesco Scaramuzzi, ENEA, Frascati (retired), Italy. Mahadeva Srinavasan, BARC (retired), India. Edmund Storms, Lattice Energy, LLC, USA. William Collis, ISCMNS. Jean Paul Biberian, University of Marseilles Luminy, France (Chairman, ICCFll). Yuri Bazhutov, Institute of Terrestrial Magnet, Russia (Chairman, ICCF13). Sponsors of ICCF12 ISCMNS: International Society for Condensed Matter Nuclear Science. TEET: Thermal and Electric Energy Technology Foundation. JCF: Japan CF-Research Society. All the full papers submitted for Proceedings book were peer-reviewed by the specialists from Japan. Revised drafts were edited, converted into LaTeX format and send to the publisher (World Scientific Publishing Co. Pte. Ltd., Singapore). For some of the presentations at the meeting of ICCF12, authors did not submit full papers and those papers are not included in the Proceedings book. Due to trivial mistake, a few papers submitted to ICCFll (Marseilles) Proceedings could not be included in the Proceedings of ICCFll (published by World Scientific Co, 2006). These missing papers by Dr. V. Violante group are included in the present book for compensation. Editors Akito Takahashi, Ken-ichiro Ota, and Yasuhiro Iwamura 30 June 2006

CONTENTS Preface

v 1. G E N E R A L

Progress in condensed matter nuclear science A. Takahashi

1

Summary of ICCF-12 X. Z. Li

26

Overview of light water/hydrogen-based low-energy nuclear reactions G. H. Miley and P. J. Shrestha

34

2. EXCESS HEAT A N D He D E T E C T I O N Development of "DS-reactor" as the practical reactor of "cold fusion" based on the "DS-cell" with "DS-cathode" Y. Arata and Y.-C. Zhang Progress in excess of power experiments with electrochemical loading of deuterium in palladium V. Violante, S. Moretti, M. Bertolotti, E. Castagna, C. Sibilia, F. Sarto, M. McKubre, F. Tanzella, I. Dardik, S. Lesin and T. Zilov

44

55

Anomalous energy generation during conventional electrolysis T. Mizuno and Y. Toriyabe

65

"Excess heat" induced by deuterium flux in palladium film B. Liu, X. Z. Li, Q. M. Wei, N. Mueller, P. Schoch and H. Oehre

75

Abnormal excess heat observed during Mizuno-type experiments J.-F. Fauvarque, P. P. Clauzon and G. J.-M. Lalleve

80

Seebeck envelope calorimetry with a Pd|D20 + H2SO4 electrolytic cell W.-S. Zhang, J. Dash and Q. Wang

86

Observation and investigation of nuclear fusion and self-induced electric discharges in liquids A. I. Koldamasov, H. I. Yang, D. B. McConnell, A. A. Kornilova, V. I. Vysotskii and A. V. Desyatov

97

Description of a sensitive seebeck calorimeter used for cold fusion studies E. Storms

108

Some recent results at ENEA M. Apicella, E. Castagna, L. Capobianco, L. D'Aulerio, G. Mazzitelli, F. Sarto, A. Rosada, E. Santoro, V. Violante, M. McKubre, F. Tanzella and C. Sibilia

117

Heat measurement during plasma electrolysis K. Iizumi, M. Fujii, S. Mitsushima, N. Kamiya and K.-I. Ota

133

Effect of an additive on thermal output during electrolysis of heavy water with a palladium cathode Q. Wang and J. Dash

140

Thermal analysis of calorimetric systems L. D'Aulerio, V. Violante, E. Castagna, R. Fiore, L. Capobianco, PR. Del Prete, F. Tanzella and M. McKubre

145

Surface plasmons and low-energy nuclear reactions triggering E. Castagna, C. Sibilia, S. Paoloni, V. Violante and F. Sarto

156

Production method for violent TCB jet plasma from cavity F. Amini

163

New results and an ongoing excess heat controversy L. Kowalski, G. Luce, S. Little and R. Slaughter

171

3. T R A N S M U T A T I O N Observation of surface distribution of products by X-ray fluorescence spectrometry during Z>2 gas permeation through Pd Complexes Y. Iwamura, T. Itoh, M. Sakano, N. Yamazaki, S. Kuribayashi, Y. Terada and T. Lshikawa Discharge experiment using P d / C a O / P d multi-layered cathode S. Narita, H. Yamada, D. Takahashi, Y. Wagatsuma, S. Taniguchi and M. Itagaki Producing transmutation element on multi-layered Pd sample by deuterium permeation H. Yamada, S. Narita, S. Taniguchi, T. Ushirozawa, S. Kurihara, M. Higashizawa, H. Sawada, M. Itagaki and T. Odashima

178

188

196

Experimental observation and combined investigation of high-performance fusion of iron-region isotopes in optimal growing microbiological associations V. I. Vysotskii, A. A. Kornilova, A. B. Tashirev and J. Kornilova Research into low-energy nuclear reactions in cathode sample solid with production of excess heat, stable and radioactive impurity nuclides A. B. Karabut

206

214

Influence of parameters of the glow discharge on change of structure and the isotope composition of the cathode materials /. B. Savvatimova and D. V. Gavritenkov

231

Elemental analysis of palladium electrodes after P d / P d light water critical electrolysis Y. Toriyabe, T. Mizuno, T. Ohmori and Y. Aoki

253

Progress on the study of isotopic composition in metallic thin films undergone to electrochemical loading of hydrogen M. Apicella, V. Violante, F. Sarto, A. Rosada, E. Santoro, E. Castagna, C. Sibilia, M. McKubre, F. Tanzella and G. Hubler In situ accelerator analyses of palladium complex under deuterium permeation A. Kitamura, R. Nishio, H. Iwai, R. Satoh, A. Taniike and Y. Furuyama High-resolution mass spectrum for deuterium (hydrogen) gas permeating palladium film Q. M. Wei, X. Z. Li, B. Liu, N. Mueller, P. Schoch and H. Oehre ICP-MS analysis of electrodes and electrolytes after HNO3/H2O electrolysis S. Taniguchi, S. Shimadu, H. Yamada, S. Narita, T. Odashima, N. Teshima and T. Ohmori The Italy-Japan project — Fundamental research on cold transmutation process for treatment of nuclear wastes A. Takahashi, F. Celani and Y. Iwamura

264

272

278

284

289

4. N U C L E A R PHYSICS A P P R O A C H Reproducible nuclear emissions from Pd/PdO:Dx heterostructure during controlled exothermic deuterium desorption A. G. Lipson, G. H. Miley, A. S. Roussetski, B. F. Lyakhov and E. I. Saunin Correct identification of energetic alpha and proton tracks in experiments on CR-39 charged particle detection during hydrogen desorption from Pd/PdChH^ heterostructure A. S. Roussetski, A. G. Lipson, B. F. Lyakhov and E. I. Saunin

293

304

Intense non-linear soft X-ray emission from a hydride target during pulsed D bombardment G. H. Miley, Y. Yang, A. Lipson, M. Haque, I. Percel and M. Romer

314

Enhancement of first wall damage in ITER type TOKAMAK due to LENR effects A. G. Lipson, G. H. Miley and H. Momota

325

Generation of DD-reactions in a ferroelectric KD2PO4 single crystal during transition through curie point (Tc = 220 K) A. G. Lipson, G. H. Miley, A. S. Roussetski and E. I. Saunin

336

Study of energetic and temporal characteristics of X-ray emission from solid-state cathode medium of high-current glow discharge A. B. Karabut

344

A novel LiF-based detector for X-ray imaging in hydrogen loaded Ni films under laser irradiation R. M. Montereali, S. Almaviva, T. Marolo, M. A. Vincenti, F. Sarto, C. Sibilia, E. Castagna and V. Violante Observation and modeling of the ordered motion of hypothetical magnetically charged particles on the multilayer surface and the problem of low-energy fusion S. V. Adamenko and V. I. Vysotskii

351

356

5. MATERIAL SCIENCE Evidence of superstoichiometric H/D lenr active sites and high-temperature superconductivity in a hydrogen-cycled Pd/PdO A. G. Lipson, C. H. Castano, G. H. Miley, B. F. Lyakhov, A. Yu. Tsivadze and A. V. Mitin

367

New procedures to make active, fractal-like surfaces on thin Pd wires F. Celani, A. Spallone, E. Righi, G. Trenta, G. D'Agostaro, P. Querela, V. Andreassi, 0. Giacinti, P. Marini, V. Di Stefano, M. Nakamura, F. Todarello, E. Purchi, A. Mancini, P. G. Sona, F. Fontana, L. Gamberale, D. Garbelli, E. Celia, F. Falcioni, M. Marchesini, E. Novaro and U. Mastromatteo

377

Using resistivity to measure H/Pd and D/Pd loading: Method and significance M. C. H. McKubre and F. L. Tanzella

392

Measurements of the temperature coefficient of electric resistivity of hydrogen overloaded Pd A. Spallone, F. Celani, P. Marini and V. Di Stefano

404

Magnetic interaction of hypothetical particles moving beneath the electrode/electrolyte interface to elucidate evolution mechanism of vortex appeared on Pd surface after long-term evolution of deuterium in 0.1 m LiOD H. Numata and M. Ban Unusual structures on the material surfaces irradiated by low-energy ions B. Rodionov and I. Savvatimova

411

421

6. THEORY Context for understanding why particular nanoscale crystals turn-on faster and other LENR effects S. R. Chubb

430

Models for anomalies in condensed matter deuterides P. L. Hagelstein

441

Time-dependent EQPET analysis of TSC A. Takahashi

454

Unifying theory of low-energy nuclear reaction and transmutation processes in deuterated/hydrogenated metals, acoustic cavitation, glow discharge, and deuteron beam experiments Y. E. Kim and A. L. Zubarev

462

Catalytic fusion and the interface between insulators and transition metals T. A. Chubb

473

Multiple scattering of deuterium wave function near surface of palladium lattice X. Z. Li, Q. M. Wei, B. Liu, N. N. Cai, S. X. Zheng and D. X. Cao

482

Theoretical comparison between semi-classical and quantum tunneling effect F. Frisone

494

New cooperative mechanisms of low-energy nuclear reactions using super low-energy external field F. A. Gareev and I. E. Zhidkova

504

Polyneutron theory of transmutation J. C Fisher The thermal conduction from the centers of the nuclear reactions in solids K.-I. Tsuchiya Four-body RST general nuclear wavefunctions and matrix elements /. Chaudhary and P. L. Hagelstein

516

521

527

Study on formation of tetrahedral or octahedral symmetric condensation by hopping of alkali or alkaline-earth metal ion H. Miura

536

Calculations of nuclear reactions probability in a crystal lattice of lanthanum deuteride V. A. Kirkinskii and Yu. A. Novikov

542

Possible coupled electron and electron neutrino in nucleus and its physical catalysis effect on D-D cold fusion into helium in Pd M. Fukuhara

547

Tunnel resonance of electron wave and force of fluctuation M. Ban

555

Types of nuclear fusion in solids N. Yabuuchi

564

XV

Neutrino-dineutron reactions (low-energy nuclear reactions induced by D2 gas permeation through Pd complexes — Y. Iwamura effect) V. Muromtsev, V. Platonov and I. Savvatimova

571

An explanation of earthquakes by the blacklight process and hydrogen fusion H. Yamamoto

577

Theoretical modeling of electron flow action on probability of nuclear fusion of deuterons A. I. Goncharov and V. A. Kirkinskii

582

Author Index

589

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P R O G R E S S IN C O N D E N S E D M A T T E R N U C L E A R SCIENCE

A K I T O TAKAHASfflt Osaka

University,

Yamadaoka E-mail:

2-1, Suita, Osaka 565-0871, [email protected]

Japan

Recent studies of condensed matter nuclear science (CMNS) including cold fusion have accumulated some convincing data and theoretical modeling, and we are about to conclude that (1) deuteron-related clean fusion reactions and (2) cold and special transmutations may take place in the environment of condensed matter containing deuterons and protons. This emerging field of CMNS is expected to give us strong impact on the future of basic sciences for energy-application, fundamental nuclear science, and condensed matter sciences.

1. Introduction Condensed matter nuclear science (CMNS) was born as a descendant research field of Cold Fusion. In March 1989, S. Pons and M. Fleischmann at University of Utah announced "cold fusion" by D 2 0 / P d electrolysis in test tube. The experimental system looked very simple. So many people in the world were involved in hurried trials of replication-experiments. In most trials, however, huge excess heat as claimed by Pons-Fleischmann was not observed. Parallel replication trials for the Nature paper by S. Jones on weak 2.45 MeV DD neutron emission from D20/Ti electrolysis cell were not either successful. Very negative mood was seen in almost all scientific communities in the world. 1 In 1990-1992, some hopeful data on excess heat in D 2 0 / P d cells were reported from research teams in USA, Japan, and Italy. Although reproducibility was yet to be attained, great expectation was come back for the clean energy application based on "new nuclear energy process". In Japan, the New Hydrogen Energy (NHE) project was implemented in 1994-1998, at Shin-Sapporo Laboratory, where about 20 researchers from major Japanese industries and several foreign scientists worked together to verify the excess heat effect in Fleischmann-Pons type systems. The NHE effort was concentrated in D/H absorption data in metal-samples and excess heat detection. In spite of energetic efforts by the NHE team, they made final report that excess heat effect was not confirmed. Few positive data on excess heat from foreign researchers and some positive data on nuclear products from Japanese University teams were unfortunately not meaningfully evaluated by the NHE evaluation committee. The NHE project was terminated in 1998. tSubmitted for keynote paper in ICCF12, November 2005. 1

2

In 1999, Japan CF-Research Society (JCF) was founded for minimumsupporting of research activities in Japan. JCF meetings (JCF1-6) held annually have provided opportunities of exchanging hottest results and accumulating reports in its Proceedings. A faint but steady stream of CF researches has continued in the world after 1990. ICCF-series conferences have counted 11 meetings (ICCF1-ICCF11). The last ICCF conference (ICCF11) was held in Marseilles, November 2004. Other smaller international meetings have been held as Asti-series workshops, Russian cold transmutation conferences, sessions at ANS and APS, and so on. It is thought with rough statistics that about 300 researchers in the world have been continuing CMNS/CF studies. Accumulated research reports are piling up high, as published in ICCF Proceedings, 2-4 Asti-Proceedings, 5,6 and so on. Unfortunately, publication of papers on CMNS/CF works has been rejected by many of highly ranked magazines and journals as Nature, Science and Physical Review Letters, but many peer-reviewed papers have been published in Fusion Technology, Japanese J. Applied Physics (JJAP), Physics Letters A, J. Electro-analytical Chemistry, II Nuovo Cimento, and so on. In the end of 2003, re-evaluation of CF works was done by US DoE, 8 based on the report by Hagelstein et al.7 The DoE report concluded that excess heat effect was not confirmed although the continuation of research was necessary. Latest progress by research reports in 2001-2005 takes over the summary report, 7 and convincing results are given for concluding the existence of excess heat effect with 4 He generation and selected nuclear transmutations. In March 2004, CMNS/CF researchers have at last founded the International Society for Condensed Matter Nuclear Science (ISCMNS) registered in England. This is the first international society for CMNS/CF researchers, which will play a role as host society of international meetings as ICCF and Asti-series workshops and exchange information through its web-site http://www.iscmns.org/ for ISCMNS members and related people. The sustainable development is now widely regarded to be a way of human beings in the 21st century. To solve the energy problem, the idea of best mixing of various available energy sources may be a compromised solution. To mitigate the pollution of environment, cleaner energy resources are being looked for. Solar energy and windmills can merely cover a small portion of energy needs. Extension of nuclear power plants is on the dead lock due to accidents and expensive processing of wastes. Development of thermo-nuclear fusion reactors is also on the dead lock due to the monstrous expensive machine. Some (and probably many) people are seriously dreaming the realization of portably small clean power sources based on some new principles, especially the idea of clean and small-scale source of nuclear energy which can be distributed in private houses and with vehicles (see Slide 1). The emerging field of CMNS including cold fusion is therefore of great potential importance.

3

Energy is key for sustainable development of world Oil: 50-60 years (COa global warning) Solar-E, wind: ca. 10% of E-needs is limit U (235) fission: 50-60 years for LWRs FBR (Pu): ca. 500 years or more (Rapid development of China and India) (Problem in remediation of nuclear wastes) DT fusion: not available PRs in 50 years Distrlbuted-type clean nuclear energy devices are ideal

Slide 1 Slide 2 shows the known fusion reactions by hydrogen isotopes. DD reaction was originally considered as fundamental reaction in cold fusion, but claimed experimental results have revealed that condensed matter nuclear effects (CMNE) are quite different.

Fusion reactions are E-source in universe H + H

D + p+ + y : weak interaction, star

H + D

3

He + y + 5 . 5 MeV:star

D+ D

4

He + y + 2 3 . 8 M e V ; 1 C r 5 %

p + t + 4.02MeV;50%

•

D+T

n + 3 He + 3.25 MeV; 50% n + 4 He + 17.6 MeV: hot fusion

D + Li, P + Li, P + B, etc.

Slide 2 An amount of 1 W excess power by DD reaction corresponds to 10 12 f/s reaction rate. Therefore, if excess heat by CMNS experiments were by DD reactions, experimenters should have died 1 by high dose irradiation of 2.45 MeV neutrons. On the contrary, we could have found only very weak level of neutrons in CF experiments. 2-4 We have had to consider new class of nuclear reactions, probably

4

related to deuterons, in the environment of condensed matter. Some of theoretical models recently developed have proposed mechanisms to produce cleanly 4 He main ash and selected transmutations in metal-D/H systems as discussed later in this report. In frontiers of science pursuing new phenomena, combined actions between Experimentalism, Rationalism, and Skepticism should support the progress. Aspects to application of the phenomena are also important. 1. Experimentalism: The effect should be reproducible with same conditions, qualitatively and quantitatively. Qualitative repeatability of phenomena by other methods and/or other groups is "broadened" reproducibility; the phenomenon with excess heat with 4 He production has cleared this criterion. To be perfect, quantitative reproducibility is required: The technological application is only possible by clearing this criterion. 2. Rationalism: Theoretical models should be created with original ideas. New theories should be compatible to established theories and should be selfconsistent within own theoretical model. All contradictions should be cleared. 3. Skepticism: Defects and contradictions in experiments should be attacked. Mutual consistency between experimental results, new models and established theories should be checked to find contradictions. 4. Applicability: Feasibility for R&D to distributed clean nuclear energy devices should be critically discussed. Remediation of radioactive wastes from nuclear plants should be also discussed. Most essential consequences of latest CMNS studies may be summarized into the following three items: 1. Occurrence of deuteron-related clean fusion producing excess heat and 4 He. 2. Occurrence of selective transmutations of host metal nuclei and fission-like foreign elements. 3. New theoretical models to interpret qualitatively and quantitatively above results. Major experimental results and representative authors are summarized in Slide 3. Major results after 1998 are considered in Slide 3. Items (1) and (2) are independent of known DD reaction and should be new kind of nuclear reactions, but items (3) and (4) are closely related to the occurrence of cold fusion phenomena. 2. Generation of Excess Heat and 4 H e in Metal-D Systems Processed metal (mostly Pd) test samples with nano-technology have recently been used for heavy-water electrolysis, D2-gas permeation and gas-discharge experiments. Experiments with heavy water are no longer simple test tube-type, but various kinds of stimulation techniques have been tried as slow and fast pulsed electrolysis-current supply, ultra-sonic wave supply, laser-beam supply, plasma-mode-electrolysis, and so on.

5

Major experiments (green; after 2001)

1) Excess heat with He-4 Miles,

, McKubre, Gozzi, Isobe, , and so on , Mizuno, Miley, Ohmori, , and so on

3) Weak neutron emission , Takahashi, Mizuno, and so on

4) Anomalous DD enhancement , Takahashi, Huke, and so on Slide 3 The nano-modification of sample, especially surface modification is of current trend of experimental innovations as well as nano-particles, complex multi-layers, micron-size long wires, and so on. Positive and convincing data have been reported from Israel + SRI + ENEA group, 9 ' 10 Arata, 1 1 - 1 5 McKubre, 16,17 de Ninno, Celani, NRL-San-Diego, Li, Case, Cravens, Isobe, 18 and so on. Key issues in experiments are calorimetry, massanalysis, nano-size-condition of sample, stimulation and triggering, diagnostics, and detection. El Boher et al.9'10 have reported clear excess heat data with 25 times out put lasting long time (17 h typically) using super-wave electrolysis (see Fig. 1). They processed surfaces of sample Pd-cathodes by argon or hydrogen plasma etching. Photograph images by SEM showed finer grain sizes for argon plasma etching. They suggest condition of surface processing relating to success of excess heat. Superwave for ultrasonic wave was modulated with special wave forms programmed by computer (PC). Averaged frequency was about 20 kHz. Arata and George are doing irradiation of ultrasonic waves to Pd samples in heavy water, with simple sinusoidal function of about 20 kHz. It is interesting how the highly fractal wave form by El Boher et al. may effect on dynamic behavior of deuterons in PdDx lattice systems. One of their collaborators is asserting that superposition of superwaves in microscopic limit can induce microscopic ordering of condensed matter and bio-systems and induce nuclear reactions. Effect on ordering in atomic or molecular size level should be interesting, but phonon or electromagnetic wave should not so easily induce directly nuclear reactions.

In series of their experiments they reported large excess power reaching more than 10 times of input power for time-spans of more than several hours. Reproducibility is in 20-30%. Best data are shown in Fig. 1, where 20 W averaged output with 0.74 W input lasted for 17 h. Gain was 25! This excess power level is corresponding to 24.8 keV per Pd-atom-in-lattice, and is far greater (more than 1000 times) than chemical heat source level.

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Excess power up to 34 W; average -20 W for 17 h Figure 1.

Best output-power data obtained by El Boher et al.

This group is trying superposed stimulation with laser beam and ultrasonic wave. This is interesting trial. The group has obtained data for 4 He production in correlation with excess heat generation. An example of data is shown in Fig. 2. When we irradiate laser on surface of Pd cathode, we can choose laser wavelength in ultraviolet and EUV region due to the classical Drude formula for frequency dependence of dielectric constant of metal. They used He-Ne laser (632 nm wavelength). Also they observed increase of excess power of several times of laser input power (33 mW). On the right-hand side figure of Fig. 2, time-dependent data of relative resistance ratio of PdDx are drawn. During the laser irradiation and excess power episode, D/Pd ratio kept more than 0.9. However, continuation of laser irradiation induced no excess power and decrease of D/Pd ratio (increase of resistance ratio). This is very interesting data showing relation between excess power and D/Pd ratio under laser stimulation. Arata et al.11^15 have made significant contribution to provide clear experimental data of 4 He production from their own double structure cathode of Pd in heavy water electrolysis cell and from D-gas-phase absorption system of Pd nano-particles

7

under laser or ultrasonic wave irradiation. Their 4 He analysis by QMAS is reliable. Detection of neutron emission was tried in-situ, but could not observe meaningful events. Tritium production in electrolyte liquid was checked periodically for sampled heavy-water by LSC to observe no significant increase of tritium level compared with BG sample. They observed great amount of 4 He from Pd powder by heating. Arata et al. also tried laser irradiation experiment on Pd nano-particles (5 nm in diameter) in ZrO substrate, and observed clear 4 He generation. 11,15 This experiment gave important hint to theoretical modeling 57 of CMNE in finite size PdDx lattice system. Violante: SIENA 2005

3.4 kJ of produced energy: 2.5 MJ/mol Pd 632 nm (He Ne), 33 mW Laser-off

Excess of power under laser triggering

Loading evolution

(laser off effect). Hi-Lo current mode

(normalized resistance)

Figure 2. Excess power data triggered by laser (left figure) and variation of resistance ratios (right figure), after Violante et al.

McKubre et al. in S R I 1 9 - 2 1 have made great efforts in replicating experiments by Arata and Case. 19 They were also involved in their own systems of closedtype heavy-water/Pd electrolysis to detect excess power and 4 He and their mutual correlation. Data shown in Fig. 3 were taken in Case-type cell, which employed PVC-deposited Pd layer on carbon. Produced 4 He goes out partially into gas-phase of cell, and other portion will be remained in Pd cathode. They collected both components and made He analysis. They obtained correlation data as 31 MeV per He-atom with 13 MeV error bar. This is important data indicating that ash of excess heat events was 4He-nuclei. George et al.23 have been studying the effect of excess heat with 4 He production using the ultra-sonic wave irradiation into Pd-plate in heavy-water, and reported

8

that the effect is real. It was observed that Pd-plate was destroyed into small powders during the experiment. Stringham 24 has been studying the similar method with higher frequency (in MHz range) ultrasonic wave. We have other reports on 4 He production by de Ninno, Isobe, 18 and so on. We can say that the phenomenon of excess heat with 4 He generation is "qualitatively" reproducible. However, conditions for 100% reproducible protocols are yet to be established. To find quantitatively reproducible conditions, we need investigations on nanomodification of samples, procedures to keep high D/Pd ratios and dynamic D-flux through samples and external stimulation methods (electrolysis patterns, laser and ultra-sonic wave irradiations, and so on).

150 Gradient

)'=18.36X

it = 0,99 Differential

y = 18.36x f? = 0.99

100

4=

Gradient Q = 31 ± 13 MeV/atom Differential 0= 32 ± 13 MeV/atom ! ^-'

50

0 • 4 He + Lattice-energy (23.8 MeV).

(1)

However, this hypothesis has no support from nuclear physics theory as we discuss in the theory section. 3. Nuclear Transmutations in Metal-D Systems Reports claiming nuclear transmutations in CF experiments using metal-D systems have gradually increased 2-4 since around 1992. People have looked the claims of transmutations with doubtful views since transmutation should overcome very high Coulomb repulsion of two-body nuclear interactions and even cold DD reaction with milder Coulomb repulsion condition looks impossible. Nevertheless, from the latest experimental results, we have to take seriously the case of "special kinds of nuclear transmutations in the environment of condensed matter of metal-D systems".

9

Major reports 2 " 6 are from Iwamura, Mizuno, Celani, Yamada, Karabut, Violante, Miley, Mastromatteo, Savvatimova, Passel, Szpak, and so on. Key issues in experiments are mass-analysis, isotopic-ratio analysis, spectroscopic detection of particles (including X-rays and gamma-rays), nano-modification of samples, and external stimulation (or triggering). Most remarkable and reproducible transmutation experiments have been reported by MHI Iwamura group. 2 5 " 2 9 They are using Pd-complex samples which have multi-layered structure of about 100 nm surface Pd layer and following four layers of alternative CaO/Pd composition (see Fig. 4) on 0.1 mm thick Pd substrate plate. They put small amount of test elements (Cs or Sr) on surface. They set a sample in a chamber filled with 1-atom D2 gas and evacuate the volume rear sample plate. D-atoms permeate through sample by keeping permeation rate higher than 1 seem. They have made in situ analyses of surface elements by Xray-induced Photoelectron Spectroscopy (XPS) or X-ray Fluorescence Spectroscopy (XFS). Amazingly, they observed transmutations of 133 Cs -^ 1 4 1 Pr, 88 Sr -^ 96 Mo for the cases of D-permeation, but did not at all for H-permeation.

Cross section of Pd complex D permeation Cs, Ba, etc.

i..rT-"-;>T j.

Dflux Vacuum

Figure 4.

D2 gas permeation through the Pd complex.

The claimed transmutation channel is strangely selective as M{A, Z) + 4D (or 2 4 He) -> M(A + 8,Z + 4) + Q.

(2)

People have checked if there are misunderstandings in experimental procedure, contamination of impurity elements, mistakes in element and mass analyses, and others to find nothing wrong as far as they have checked through. People have started to take this result of "selective transmutation" seriously. Takahashi-group of Osaka University tried replication 30 of Iwamura experiments to result in observation of Pr production from Cs, three times out of three runs. Iwamura group has been doing separate series of experiments at Spring8 setting

10

up new chamber with incidence of strong SOR X-ray beam to make in situ FXS analysis of surface elements of Pd-complex under D-permeation. They have repeatedly observed transmutation from 133 Cs to 1 4 1 Pr (see Fig. 5). They have made sample analysis after experiments by Time-of-Flight Secondary Ionization Mass Spectroscopy (TOF-SIMS) to find that transmuted Pr distributed within about 10 nm depth from surface of Pd-complex sample (see Fig. 6). The data in Fig. 6 give insight that the transmutation reaction should have taken place in near surface region.

.....a...... 35 Cs-U;,

™, # ™>36

Iw—s* Br ^.4

Cs-L p1

1

•

4

;

T ,if

I

•

100-

1m -A

i' i

. ^

•,

i

• • i

1

' !-\

i

' V

Cs Lp2

'i*

J

50-

Energy (keV) Figure 5.

An experiment of Pr detection by the experiments at Spring-8 (Imaura, ICCF11).

To explain theoretically the surprising selective transmutation, Takahashi is developing the EQPET/TSC model of bosonized condensates of deuteron clusters under ordered dynamics of PdDx lattice, and T. Chubb-S. Chubb are proposing coherent reaction models by ion-band state of Bloch wave functions of many deuterons in lattice, as we will discuss in Section 5. When this transmutation process also takes place for radio-isotopes as 137 Cs and 90 Sr, the principle can provide a new way for remediation of nuclear wastes. Observations of anomalous production of foreign elements in D 2 0 / P d and Pd/Dgas systems have been reported by Mizuno, Ohmori, Karabut, Szpak 105 and so on. In these cases, they observed also excess heat events. Observed foreign elements are very common among these reports, namely Si, S, Ca, Ti, Cr, Mn, Fe, Cu, Zn, etc. Mizuno 31 reports that production rates of foreign elements were drastically small (several orders of magnitude) when excess heat evolutions were not observed. If these foreign elements, which were distributed in a wide range of mass and atomic number, were generated by some nuclear reaction, some fission process of host metal nuclei should be attributed to the reaction.

11

200

0

400

600

1000

800

Sputtering time (s) Figure 6.

Depth profile of Cs and Pr by TOF-SIMS (Iwamura, ICCF11).

Takahshi et a/. 32-34 have proposed a deterministic fission theory [Selective Channel Scission (SCS) model] based on rotating liquid drop model of excited nucleus. They checked the model successfully for calculating mass and atomic number distributions of fission products (FP) by 2 3 5 U+n fission process 33 to be compared with experimental data. Then they applied the model for predicting FP distributions of lower mass nuclei of A < 200. Mizuno's foreign element data are compared with Takahashi calculation in Fig. 7. Theoretically predicted element distribution looks similar to Mizuno experiment. In the SCS process, isotopic ratios of FP element become very different from natural abundances. For example, 57 Fe exists with 0.3% in natural iron, but both of FP of SCS theory and experiments by Mizuno gave similar values of about 10% in FP iron

« Fission products by theory {MPIF, Takahashi et al.) » Mizuno Exp, by D2Q-Pd/etectrolysis

100

Pd-natural LB-1

.MPIF • MIZUNO-EXP

10

1 t

Sr

0.1

0

5

10

15

20

25

30

35

40

45

50

Atomic number Figure 7. Foreign atom distribution obtained by Mizuno's D2O electrolysis, compared with theoretical prediction of Pd-fission products calculated by SCS theory by Takahashi et al.

12

isotopes. These agreements are quite interesting, and further studies are expected to verify if the phenomenon is really nuclear fission process for lighter nuclei in the environment of metal-D systems. Similar results have been reported for Ni-H systems as discuss below. The SCS theory predicts that fission products for A < 200 nuclei become very much cleaner (less radio-active and very small neutron emission) due to predominant production of stable isotopes. 3 2 - 3 4 4. Metal—Hydrogen Systems Observation of anomalous production of foreign elements and excess heat in metalordinary-water/H systems have been claimed 2 " 6 in reports by Piantelli, Ohmori, Miley, Yamada, Romadanov, Dash, Li, Mizuno, and so on. Key issues of experiments are again calorimetry, mass and isotopic analyses, radiation detection, sample fabrication, and triggering and stimulation techniques. Piantelli et al.36'37oi Siena University has been doing a H-gas absorption and diffusion type experiments using cylindrical Ni samples in chamber with heating device. They have made claim of large excess heat and gamma-ray emission with production of foreign elements. Figure 8 shows one of their typical data for observation of gamma-ray emission. They set up a standard 137 Cs gamma-ray (661 keV peak) source for calibration. The observed peak at around 744 keV is a surprise, which they say the gammaline from Mn isotope. A theoretical prediction by Takahashi's 4p/TSC-induced fission35interpret that 52 Mn and 56 Ni as FPs of Ni + 4p fission process can be sources of 744 keV line. It is well known that Miley-Patterson 38 reported distributed production of transmuted elements and excess heat in their Ni-ordinary-water electrolysis experiments.

Piantelli; SIENA 2005

Photo emission Cell with cylindrical smples

Cs source 661 keV

TARATURAconCs-137

Comment by A. T. 400.00 Mn (EC) (90%) 744.2 keV y 200.00 Ni-fl-4p-> C + "Fs(EC)"Mn(ECi"cr(EC) 0.00

1

0.00

Figure 8.

1 200.00

'

1 400.00

'

1 600-00

'

1 Canal! 800.00

Gamma-ray spectrum obtained in Ni-H-gas experiment by Piantelli et al.

13

Data from Miley'96 t

1 t.


4 He+ lattice-energy (23.8 MeV) does not have place to stand on, in the view of nuclear physics 57 (see Fig. 10).

Takahashi: SIENA 2005

d + d -> 44He*(23.8 MeV) -> break-up « Branching ratio: Sn(0)/Sp(0)/Sg(0) =

&»s/////////J< 20.577 • 19,814-

r„/r,/rg =

„ 3 © . n + aHe — -*• p +1

0.5/0.5/0.0000001 • r n = r p = 0.2 MeV • r g = 0.2 MeV

Qamma transition

• r, = r n + r p + r g .T = WT,=1E-22S

0.0-

Figure 10.

-4He(gs)

• No forces to change BRs have ever been proposed!

Final state interaction and branching ratios for d-d fusion.

In EQPET/TSC models by Takahashi, 5 0 - 5 8 the idea of bosonized condensates was substantiated. To induce 4 He production without neutron emission, he made the third and fourth hadrons (deuterons or protons) participating into d-d strong interaction. In consequence, he had to treat multi-body fusion (or cluster fusion) reactions under ordered constraint of Tetrahedral Symmetric Condensate (TSC) motion in PdDx lattice. In other ways, Chubb-Chubb 7 1 - 7 4 and Hagelstein 69 ' 70 have proposed some sort of coherent fusion processes for so-many-body systems in PdDx lattice to try to

16

2) Minimum TSC

V

A ^ 4

xr 3) Be* formation

4

He

He

4) Break up

Figure 11. Illustration of TSC squeezed condensation; (a) TSC formation at t = 0, (b) minimum size state of condensed TSC, (c) formation of 8 Be* by strong interaction, and (d) break-up of 8 Be* into two alpha-particles.

reach 4 He production channels. Takahashi treats rather microscopic coherence, while Chubb-Chubb and Hagelstein do rather macroscopic coherence in metaldeuterium lattice systems. In theorizing nuclear effects in CMNS, to point out qualitatively new reaction channels is not enough at all. We have to quantify theoretical models to show quantitative (numerical) predictions that new reaction channels will be feasibly taken place. For example, such reaction channels as D + D —>4 He + 7 (23.8 MeV) or 133 Cs + 4D -^ 1 4 1 Pr + Q (50.49 MeV) look possible from the mass-energy conservation of Einstein relation, because of exothermic reactions, but actually these do Strong F. Bare Coulomb potential

Figure 12. Shielded Coulomb potential for dde* pseudo-molecule under steady-state assumption; relation to screening energy and strong interaction range for d-d reaction is illustrated.

17 Table 1. Screening energy of E Q P E T molecules Us = e2/b0 for V3 (b0) = 0 (Takahashi, SIENA 2005). Us(eV)

e*

(1.1) (2.2) (4,4) (8,8) (208,1)

b0 (pm)

dde*

dde*e*

dde*

dde*e*

36 360 4000 22154 7579

72 411 1108 960 7200

40 4 0.36 0.065 0.19

20 3.5 1.3 1.5 0.20

not happen unless high potential barriers of Coulomb repulsion can be overcome by particular ways that we should theorize. We have to estimate how Coulomb repulsion is overcome in the initial state interaction, how intermediate compound state is and what are branching ratios in the final state interaction. Theoretical modeling should be self-consistent so as to be quantified. The theory of EQPET/TSC by Takahashi 50 " 58 is trying to give quantified predictions. Recently at ICC10, Takahashi proposed TSC of four deuterons and four electrons in PdDx lattice dynamics forming a transient quasi-molecular state of orthogonally coupled two D2 molecules and squeezing semiclassically into central T-site to reach TSC-minimum-size state with about 10 fm diameter as charge neutral pseudo-particle. The TSC-minimum state for 4D/TSC causes self-fusion of 4D to 4 He + 4 He + 47.6 MeV, or capture reaction (selective transmutation) with host metal nucleus. This scenario is shown in Fig. 11. Takahashi treats transiently bosonized states of electron pairs with anti-parallel spins and quadruplet coupling e*(4,4) by Electronic Quasi-Particle Expansion Theory (EQPET). 5 1 - 5 5 He treats virtual pseudo-molecule dde* as illustrated in Fig. 12. He calculated screened potentials for dde* molecules and estimated screen energies and other potential parameters as given in Table 1. Nuclear strong force for fusion is estimated based on the concept of optical potential (see Fig. 13) and effective surface sticking force P E F 5 2 - 5 8 for multi-body (4D) fusion by TSC. • U ( r ) = V(r) + ilV(r} . l/(r) - -2.5 to -50 MeV . W(r) .0.1 to 5 MeV WW

J •4

» For fusion by surface sticking force: IV(r) - W „ 8 ( r - r 0 )

• Vs (r): screened Coulomb potential -"0

Figure 13.

Optical potential for strong interaction

18

Fusion rate in general is given for collision-like process as shown in Slide 5. ^—iment b\ A T

Fusion rate for collision process dynamic or transient process• 7= OF, |Hint| ¥i> = (Initial state interaction) x (Intermediate compound state) x (Final state interaction) • Cross-section - T2 p (E') • p (E'): final state density - Reaction-rate (ov): (4TCS//I)V72 p (E')

• (Initial) = (El. EM int) (strong int) • (Final) = BRs to irreversible decays

Slide 5 Practical formulas are given in Fig. 14. Time averaged cluster fusion rates for the TSC squeezing motion is given in Table 2. He reports some of key issues in CMNE can be explained by these EQPET/TSC models as shown in Table 3. Kim 61 ' 62 is studying CMN effects in Bose-Einstein condensation (BEC) process. He assumes that many deuterons, metal ions like Li + and electrons are confined in a void cavity in metal lattice and they are behaving as plasma. Superposition of many-body wave functions by BEC is supposed to play role for strong enhancement of dd fusion and d-6Li fusion (source of 4 He generation). Deuteron is a boson. To

F l J S i O n T a t e Of D - C l U S t e r |Takahasni:racemRes.Devel.Physics,6(2005) 1

© D-cluster formation process:

U0 = e2/r

FnD = 0F12>(4'22>Cl'32>-vI'„2> © Barrier penetration process: PB = exp (-nr„) Screened potential

® Nuclear fusion process: a = SnD/Ed !_ = av* PB* FnD D •!• (D +• {D -i- D)) =* 4D

For T-matrix elements: (1) and (2): EM interaction, (3): strong interaction Figure 14. Three-step Born-Oppenheimer treatments in formulating D-cluster fusion rates in condensed matter.

19 Table 2. e* (m, Z) (1,1) (2,2) (4,4)

T D E Q P E T calculation for E Q P E T molecules (Takahashi, ICCF12).

(A 2d) (f/s/cl.) 44

4.3 x 1 0 2.9 x 1 0 " 2 5 2.1 x 10~ 1 7 *

(A Ad) (f/s/cl.) 7.8 x 10" 2.5 x 10" 5.5 x 10"

A 2d (0) (f/s/cl.) 60

1.9 x 1 0 " 2.4 x 1 0 ~ 3 7 5.5 x 10" 2 2 *

A 4d (0) (f/s/cl.) 7.3 x 1 0 ~ 9 3 1.1 x 10~ 5 0 5.9 x 1 0 " 2 0

*Virtual value.

minimize system Coulomb energy of particles in the cavity should, however, lead to charge neutralization between deuterons and electrons to form D-atoms for dilute gas (or D2 molecules after collision process for dense gas). Plasma state at room temperature looks no good idea. And D-atoms are fermions due to odd (non-integer) spin for electron. Models by Kim and Tsuchiya need further elaboration. Takahashi's EQPET/TSC models are kind of bosonized condensate models. However, TSC is bosonized condensate under strong constraint (namely ordering process in lattice), different from BEC of dilute gas at near zero temperature but similar to bosonization of fermions (formation of Cooper pair) for super-conductivity and super-fluid. New aspect as CMNS is "Bosonization in Ordering Process". X. Z. Li has studied Resonant Tunneling Model. 64 ' 65 Intermediate compound state of fusion reactions in CM may have, he proposes, excited state with very long (as 104 s) life time to select resonating decay channel for final state interaction. During his study he has made nice progress to fit fusion cross sections for DD, DT, and D 3 He reactions using revised formulas of elementary phase-shift analysis of scattering matrix and optical potential. This is good progress. However, his model cannot change the situation of Fig. 10, namely for drastically increase branching ratio to 4 He channel since longer life time makes the gamma-transition branching ratio smaller. Hagelstein has been studying a kind of coherent fusion model to explain neutronless 4 He generation and excess heat. His models do not reach the stage of quantified theory, but are trying to approach to quantification. Recently he is proposing the phonon-coupled gauge models, assuming 'compact' intermediate state of (n-3He) to evaluate gauge transform between (d-d) state, (n-3He) state, and irreversible Table 3.

Major results: experiments versus theory.

Item

Experiment Author/Method/Results

E Q P E T / T S C model

Screening

Kasag/beam/310 eV Takahashi/3D/10 9 (dd) McKubre/electrolysis/ 30±13MeV/4H El Boher/EI/24.8 keV/Pd, Gain = 25 Iwamura/Perm/Cs —> Pr Miley/NiH/Fission-like Pro.

360 eV by dde* (2,2) (10 1 3 ) r (0.1 ms)

He production Maximum heat Transmutation

23.8 MeV/ 4 He by 4D - • Hex2 + 47.6 MeV 23 keV/Pd 46 MeV/cc by 4d/TSC 4d/TSC + M 4p/TSC + M reaction 4

20

out-going channel to 4 He. This is an elegant approach. However, there are some fundamental problems. First, (n-3He) state may not exist with meaningfully large life time to be prohibited to going out to the n + 3 He + 3.25 MeV channel with very short life time (on the order of 10~ 22 s) from the intermediate compound state 4 He* as shown in Fig. 10. He estimates that the transform strength (QM flow) between states by phonon exchange is on the order of 1 0 - 4 , which is right but is much smaller than field coupling between strong interactions (see Slide 6, accordingly). Branching ratio to electromagnetic transition (decay channel to 4 He) cannot be increased by more than 10~ 4 of those (0.5) for n + 3 He or p + t channels. Chubb-Chubb 7 1 - 7 4 have proposed a kind of coherent fusion model through the D-ion-band state in PdDx lattice Bloch potential. They assume that QM waves of many deuterons inside a well of many-body (more than 10,000 Ds) potential can link widely and, due to the double Bloch symmetry conditions, Coulomb repulsions between deuterons eliminate in scale of 1/Nwell for Nwell more than 10,000. They also assume this coherent condition should change the intermediate compound state (4He*) of DD interaction to form 4 He-ion-band state with long life time, for which we can use wave-function form of 4 He. This is another elegant theory. To reach quantified predictions by this theory, we need to substantiate many things; to prove definitely the 1/Nwell law, to Relative strength of interactions Comment by AT.

• Nuclear strong interaction: f/hc = 1 • Electro-magnetic interact: eVhc = 7.3E-3 • Weak nuclear interaction: (ghc)2 (mc/h)4 = 5E-14 • Gravity: GM2/hc = 2E-39 . Sdd = 1.1E2 keVb versus Spp = 1E-22 keVb a ~ (T-matrix)2

Slide 6 quantify ion-band state excitation functions, to evaluate life time of 4 He-ion-band state if at all, to propose an intermediate compound state (4He*) with quite different spin-parity state through the interaction with electromagnetic Bloch potential (actually phonons by lattice vibration, harmonic oscillators, for example) to avoid final state irreversible decays to n and t channels in Fig. 10. Elaboration will be tough. We summarize elaborations for quantification of theories in Slide 7, including other models by Hora's 76 swimming electron layer model, Fisher's poly-neutron model and Kozima's neutron-catalyzed reaction model.

21

We need quantification of models (difficult) by improving » Chubb-Chubb: is 1/N well screening by variational principle correct? We need quantitative estimations of T-matrix-components, for intermediate and final states. Can 4He-ion-band have life GT. 1E-22 s of 4He* (23.8 MeV) * Hageistein: branchinh ratio (1E-4) in competition of EM-force and Strong force is ignored? Does the compact n-3He state exist with meaningful life time? * Li: theory only treats S-matrix 9 (phase-shift analysis), hence total reaction cross-section improved. Others are speculations for final state interactions. * Fisher: no reason for polyneutron binding force found? * Hora: usage of reaction rates for random plasma is wrong * Kozima; no neutrons exist, neglect phonon-n inelastic scattering which escapes Bragg condition, wrong formula for secondary charged particle reactions, etc.

Slide 7 6. Theories with Weak Interactions and Others Interesting theoretical models are as follows: 1. Mini-H-atom (by heavy electron) formation to zero-momentum neutron model: Widom. 78 2. Mini-H-atom (by suborbital QM state): Mils,79 Yamamoto, 80 and 81 Filimonov. 3. Poly-neutron reaction model: Fisher 82 and Kozima. 83 Here key issue will be how reaction rates via weak interactions can be enhanced. Quantitative predictability is the key. Brief scenario of Widom's theory is; on the flat surface of metal-hydride, coherent coupling between many-body electron oscillations and proton oscillations makes effective electron mass significantly heavy. Mini-atom orbit of H-atom with heavy electron forms. Electron capture process into proton may be very strongly enhanced to generate near-zero-momentum neutrons. These very low-energy neutrons will be absorbed within very short range near surface to induce neutron-induced reactions. This kind of theory has many fundamental problems as: (1) Production cross section of "heavy electron" e* is not given, so that we cannot argue on density of very-low-momentum-neutron (VLMN) available in matter, taking into account of 10 min beta-decay of neutrons and assumed neutron-conversion cross section (see 3). If neutron density were greater than 1016 per cm 2 on surface, neutron reaction rate with H and host metal-nuclei were realistic level as experiments claim. According to neutron decay and

22

(2)

(3)

(4)

(5)

(6)

(7)

inelastic phonon-scattering with lattice vibration, which is up-scattering to higher neutron energy, we need to estimate mean existing time of VLMN on surface. (The author guesses that VLMNs get phonon energy with several barns of cross-section and very rapidly - in less than one micro-second-leak out from system.) Proton (deuteron) on metal surface lattice vibrates with (l/2ir) hu, as Einstein oscillator, and has "recoil energy" of about 30 meV. VLMN converted from proton should conserve this 30 meV as kinetic energy which is a little more than averaged (thermal equilibrium) energy of 25 meV in media at room temperature. (Einstein oscillator can have higher zero-point energy than Debye oscillators of metal atoms.) Cross section for p + e* to n+neutrino is not given. The author thinks this cross-section (over threshold energy of reaction) should be very much small, of the order of 1 0 - 2 6 of usual strong interactions. And neutrino here is different from electron-neutrino and muon-neutrino, and deviates from the three generations scenario of leptons. This cross-section (or transition matrix) estimation is key problem for making their theory realistic! 6 Li + n to 4 He + 1 + 4.8 MeV channel has about 1000 barn at En = 25 meV, compared with very small cross section 4 x 10~ 2 barn for n-capture, 6 Li + n to 7 Li + gamma. And 7 Li + n to 8 Li to 8 Be + beta to 4 He + 4 He + e process has 4 x 10~ 2 barn at En = 25meV, only. So, it is well known that 6 Li + n to 4 He + t + 4.8 MeV is predominant channel! Since reaction rate per neutron flux is (cross-section) x (velocity) and cross-section at lower energy than 30 meV has 1/v law, all reaction rates keep constant according to the change of momentum or kinetic energy. So that, even at very much low energy, reaction rate does not increase so. Widom-Larson might misunderstand these points. If p + e* state exists, it should have transition to mini-atom orbit which should emit photons greater than 13.6 eV of H-atom ground state. (This has some sort of relation to Randi Mill's sub-orbital quantum state, hydrino!) We need to estimate life time of e* becoming heavy by Widom's oscillating electro-magnetic plasmon (surface polariton) interaction on surface. If hard gamma-rays were totally absorbed by e*, we can do easily test using a standard gamma-ray source to measure gamma-peak attenuation through the sample metal-hydride surface. We have no data for Compton scattering with e*, which he assumes very much large to neglect gamma-electron processes with metal-atoms having usually much larger photoelectric, Compton and pair-creation cross sections compared with those for hydrogen atom. We know, dde*(mass = 208m-electron), namely muonic dd-molecule does not emit low-energy neutrons (but 2.45 MeV neutron by d-d fusion), although Widom theory suggests dde* to d + n + n break-up.

23

We can make such skeptical critics easily for other models also. By making clear every question, one by one, one can improve m o d e l s 8 4 - 8 9 and approach t o the target. We need tough efforts of elaborations. 7. C o n c l u s i o n s 1. Recent results of CMNS studies show very important consequences of Clean Fusion and Cold Transmutation. 2. We are in Turning Point for studying deeper and establishing new field of Condensed M a t t e r Nuclear Science (CMNS). 3. New progress is expected at this conference of ICCF12. References 1. J. R. Huizenga, Cold Fusion, The Scientific Fiasco of the Century (University of Rochester Press, USA, 1992). 2. Proceedings of ICCF9, Tsinhua University Pub. (2003). 3. Proceedings of ICCF10, World Scientific Pub., to be published, see also internet version at http://www.lenr-cana.org/ 4. Proceedings of ICCFU : World Scientific Pub., to be published, see also internet site http://www.iscmns.org/ 5. Proceedings of ASTI5 Meeting, see internet site http://www.iscmns.org/ 6. Proceedings of SIENA2005 Workshop, see ibid. 7. P. Hagelstein, M. McKubre, D. Nagel, T. Chubb, and R. Heckman, New Physical Effects in Metal Deuterons, Reprot to US-DoE (2003). 8. US-DoE: Report of the Review of Low Energy Nuclear Reactions, December 1, 2003, see to find paper at http://www.newenergytimes.com/ 9. El Boher et al, Proceedings of ICCF11, see Ref. 4. 10. V. Violante et al, Proceedings of SIENA 2005 Workshop, see Ref. 6. 11. Y. Arata et al, II Nuevo Saggitore 20, 66-71 (2004). 12. Y. Arata et al, JJAP 37 (11), L1274 (1998). 13. Y. Arata et al, JJAP 38 (7), L774 (1999). 14. Y. Arata et al, JJAP 39 (7), L4198 (2000). 15. Y. Arata et al, J. High Temp. Soc. Japan 29, 1-40 (2003). 16. M. McKubre et al, Proceedings of ICCF10, see Ref. 3 17. M. McKubre et al, Proceedings of ICCF11, see Ref. 4 18. Y. Isobe et al, JJAP 4 1 , 1546 (2002). 19. L. Case, Catalytic fusion of deuterium into helium-4, Proc. ICCF7, Vancouver (1998). 20. M. McKubre et al, Excess power observations in electrochemical studies of the D / P d system, Frontiers of Cold Fusion, Proc. ICCF3, Nagoya (1992), see http://www.lenrcanr.org/ Library. 21. M. McKubre et al, Development of advanced concepts for nuclear processes in deuterated metals, EPRI-Report (1994), see http://www.lenr-canr.org/ Library. 22. Y. Isobe et al, JJAP 4 1 , 866-870 (2002). 23. R. George, see Ref. 6. 24. R. Stringham, 1.6 MHz sonofusion device, Proc. ICCF11, see Ref. 4. 25. Y. Iwamura et al JJAP 4 1 , 4642 (2002). 26. Y. Iwamura et al, Proc. ICCF10, see Ref. 3. 27. Y. Iwamura et al, Proc. ICCF11, see Ref. 4.

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28. M. Sakano et al, Confirmation of transmuted elements on Pd complexes using D2 gas permeation method, Proc. JCF-5, see http://wwwcf.elc.iwate-u.ac.jp/jcf/ 29. Y. Iwamura et al, Correlation between deuterium flux through Pd complexes and quantity of nuclear products using D2 gas permeation method, ibid. 30. T. Higashiyama et al, Proc. ICCF10, see Ref. 3. 31. T. Mizuno, Nuclear Reactions in Solid, No.l, Chapter 8 (Kokakusha, 1999). 32. A. Takahshi et al., JJAP 4 1 , 7031-7046 (2001). 33. M. Ohta and A. Takahashi, JJAP 42, 645-649 (2002). 34. M. Ohata and A. Takahashi, Proc. ICCF10, see Ref. 3. 35. A. Takahashi, Theoretical backgrounds for transmutation reactions, ppt slides for Sunday School of ICCF10, see http://www.lenr-canr.org/ Special Collection for ICCF10. 36. F. Piantelli, Hydrogen loading of Ni and related phenomena, Proc. Siena2005 Workshop, see Ref. 6. 37. V. Montalbano et al, Evidence of radiation from Ni-H system, Proc. ICCF11, see Ref. 4. 38. G. Miley and J. Patterson, J. New Energy 1, 5 (1996). 39. A. Takahashi, TSC-induced nuclear reactions and cold transmutations, Proc. Siena2005 Workshop, see Ref. 6. 40. T. Mizuno et al., Hydrogen evolution by plasma electrolysis in aqueous solution, JJAP ±A, 396-401 (2005). 41. T. Mizuno et al, Proc. JCF6, Tokyo (2005), see http://wwwcf.elc.iwate-u.ac.jp/jcf/ 42. F. Celani et al, Proc. ICCF11, see Ref. 4. 43. F. Celani et al, Proc. JCF5, see http://wwwcf.elc.iwate-u.ac.jp/jcf/ 44. F. Celani et al, Proc. JCF6, see ibid. 45. V. Masteromatteo et al, Proc. Siena2005 Workshop, see Ref. 6. 46. A. Karabut et al, Proc. ICCF10, see Ref.3. 47. H. Yamada et al, Proc. ICCF10, see Ref. 3. 48. H. Yamada et al., Proc. JCF5, see http://wwwcf.elc.iwate-u.ac.jp/jcf/ 49. S. Narita et al., ibid. 50. A. Takahashi, Condensed matter nuclear effects, Proc. Int. Meet. Frontiers of Physics, Kuala Lumpur, 25-29 July 2005, Malaysian J. Physics, to be published. 51. A. Takahashi, Deuteron cluster fusion and related nuclear reactions in metaldeuterium/hydrogen systems, Recent Res. Devel. Phy. 6, 1-28 (2005), ISBN: 817895-171-1. 52. A. Takahashi, Proc. ICCF9, pp. 343-348, see Ref. 2. 53. A. Takahashi, Mechanism of deuteron cluster fusion by EQPET model, Proc. ICCF10, see Ref. 3. 54. A. Takahashi, Proc. JCF5 and 6, see http://wwwcf.elc.iwate-u.ac.jp/jcf/ 55. A. Takahashi, Proc. ICCF11, see Ref. 4. 56. A. Takahashi, Deuteron cluster fusion and ash, Proc. ASTI5 Meeting, see Ref. 5. 57. A. Takahashi, A theoretical summary of condensed matter nuclear effects, Proc. Siena2005 Workshop, see Ref. 6. 58. A. Takahashi, Time-dependent EQPET analysis of TSC, Proc. ICCF12, Yokohama (2005). 59. V. Kirkinskii and Y. Novikov, Proc. ICCF9, pp. 162-165, see Ref. 2. 60. V. Kirkinskii and Y. Novikov, Numerical Calculations of Cold Fusion in Metal (Novosivirsk University Press, 2002). 61. Y. Kim, Proc. ICCF11, see Ref. 4. 62. K. Tsuchiya, ibid.

25 63. 64. 65. 66. 67. 68. 69. 70. 71. 72. 73. 74. 75. 76. 77. 78.

79. 80. 81. 82. 83. 84. 85. 86. 87. 88. 89. 90. 91. 92. 93. 94. 95. 96. 97. 98. 99. 100. 101. 102.

K. Ttsuchiya, Proc. JCF5 and 6, see http://wwwcf.elc.iwate-u.ac.jp/jcf/ X. Z. Li et al., Proc. ICCF9, pp. 197-201, see Ref. 2 X. Z. Li et al, Phys. Rev. C 6 1 , 24610 (2000). X. Z. Li et al, Laser and Particle Beams 22 (4) (2004). X. Z. Li, Lecture at Sunday School of ICCF11, see Ref. 4. P. Hagelstein, Proc. ICCF9, see Ref. 2. P. Hagelstein, Proc. ICCF10, see Ref. 3. P. Hagelstein, Proc. ICCF11, see Ref. 4. S. Chubb, Proc. ICCF10, see Ref. 3. S. Chubb, Proc. ICCF11, see Ref. 4. T. Chubb, Proc. ICCF10, see Ref. 3. T. Chubb, Proc. ICCF11, two papers, see Ref. 4. H. Hora et al, Proc. ICCF9, p.135, see Ref. 2. H. Hora et al, Proc. ICCF10, see Ref. 3. H. Hora et al, Proc. ICCF11, see Ref. 4. A. Widom and A. Larson, Ultra low momentum neutron catalyzed nuclear reactions on metallic hydride surfaces, private communication (2005), see http://arxiv.org/abs/cond-mat/0505026 R. Mills et al, IEEE Trans. Plasma Set. 3 1 , 338-355 (2003). H. Yamamoto, Proc. JCF5, see http://wwwcf.elc.iwate-u.ac.jp/jcf/ B. Filimonv, Proc. Siena2005 Workshop, see Ref. 6. J. Fisher, ibid. H. Kozima, Proc. JCF-5, see http://wwwcf.elc.iwate-u.ac.jp/jcf/ F. Gareev, Proc. ICCF11, see Ref. 4. F. Gareev, Proc. SIENA2005 Workshop, see Ref. 6. T. Sawada, Proc. ICCF11, see Ref. 4. T. Sawada, Proc. JCF5, http://wwwcf.elc.iwate-u.ac.jp/jcf/ F. Frizone, Proc. ICCF11, see Ref. 4. V. Vysotskii, ibid. J. Kasagi et al, J. Phys. Soc. Jpn. 7 1 , 2881-2885 (2002). J. Kasagi and H. Yuki, JPSJ 58(3), 190-194 (2003). J. Kasagi et al, Proc. ICCF10, see Ref. 3. J. Kasagi et al, Proc. ICCF11, see Ref. 4. J. Kasagi, Abstract for JCF5, http://wwwcf.elc.iwate-u.ac.jp/jcf/ A. Huke, Ph. D. Thesis, Technical University of Berlin, 2004. A. Huke et al, Proc. ICCF11, see Ref. 4. A. Kitamura et al, Proc. ICCF10, see Ref. 3. A. Takahashi et al, Phys. Lett. A 255, 89 (1999). Y. Isobe ., see Ref. 22. A. Takahashi et al, Studies on 3D fusion reactions in TiDx under ion beam implantation, Proc. ICCF10, see Ref. 3. A. Takahashi et al, Fusion Technol 34, 256-272 (1998). S. Szpak et al, Evidence of nuclear reactions in the Pd lattice, Naturwissenschaften 00:1-4 (2005).

S U M M A R Y OF ICCF-12

X I N G Z. LI Department

of Physics, Tsinghua University, Beijing E-mail: [email protected]

100084,

China

The progress of the Condensed Matter Nuclear Science reported during ICCF-12 is summarized with emphasis on reply to the DOE review in 1989 and in 2004. The 18 reviewers might not be aware of the new achievement in the Advanced Technology Research Center, Mitsubishi Heavy Industries; hence, their conclusion should have been more positive toward this research. Arata's DS-reactor and the "heat after death" experiment should change the conclusion about the "excess heat" and its prospect. Various fundamental researches have shown the consistent nature in understanding. A cost effective and comprehensive study is mentioned.

1. From 1989 DOE Review to 2004 DOE Review ICCF-12 is a good chance to check the progress in the past 16 years. DOE reviews in 1989 and in 2004 represent two milestones. In the Blue Cover Book written by DOE 1989 ERAB, 1 the fifth point in conclusion was "Nuclear fusion at room temperature, of the type discussed in this report, would be contrary to all understanding gained of nuclear reactions in the last half century; it would require the invention of an entirely new nuclear process." It is true that 16 years study has confirmed that there is an entirely new nuclear process. The title of Mckubre and Hagelstein's report was just "New Physical Effects in Metal Deuterides." 2 Among the 18 reviewers, one-half of them recognized that "evidence for excess power is compelling;"3 however, only one of them recognized that the occurrence of low energy nuclear reactions is demonstrated by the evidence presented. If DOE allowed more time for the reviewers to become acquainted with the nuclear transmutation work, the other 17 reviewers might recognize also that the occurrence of low energy nuclear reactions is demonstrated, because in the past 10 years Dr. Iwamura just did what they recommended, i.e. "the use of state-of-the-art apparatus and techniques to search for fusion events in thin deuterated foils."4 2. Nuclear Transmutation in Super-Lattice Complex Dr. Iwamura's pursuing led to his great success. He started his research when Japanese New Hydrogen Energy (NHE) Project was initiated in 1993; however, he did not stop when NHE project stopped. He did not insist to use neutron as the only one signal for nuclear reaction. He tried tritium, X-rays, and excess heat. He tried both electrolysis and gas-loading method. Eventually, he found that deuterium flux, cesium coating on the surface, and the super-lattice complex were 26

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the three key elements to reproduce his discovery, i.e., the nuclear transmutation induced by deuterium flux. He found that X-ray photoelectron spectroscopy was the most suitable in-situ diagnostic tool to monitor the nuclear transmutation. His supervisor was so judicious to allow him traveling between Yokohama and Kobe in every week in order to continue his study. Indeed he was so brave to try the high Z element as a candidate to interact with the low energy deuterium gas; and he was so patient to wait for weeks in order to observe the nuclear transmutation. When his methodology was established, he was able to send his sample to France for the SIMS (time-of-flight) analysis; and send his sample to SPring-8 for microbeam analysis. Moreover, professor Takahashi of Osaka university was able to use his method to make sample, and use the Neutron Activation Analysis to verify the product of the nuclear transmutation (Pr). 5 Now Mitsubishi Heavy Industries is collaborating with Naval Research Laboratory (NRL) in US in order to use NRL's Trace Element Analysis Mass Spectroscopy equipments. The Disclose Agreement between MHI and NRL restricted the information flow before the publication; however, we might still learn from Drs. Iwamura, Narita, and Yamada's presentations. 6,7 The unidentified peak was discovered using the microbeam. Possibly, it was lanthanum (La). It was just the element between Cs and Pr. It might imply that Cs was added a deuteron first; then, one more deuteron was added to reach the Pr. Moreover, if we look at the natural abundance of lanthanum, there is only one stable isotope for lanthanum with a little mixture of long life-time isotope (0.09%, 1.05 x 10 11 years). This is very similar to the praseodymium which has only one stable isotope as well. Indeed, terbium (Tb) and thulium (Tm) were discovered in the early Electron Probe MicroAnalysis experiment also when we tried to identify any new elements in the sample of palladium hydride. 8 To my surprise, Tb and Tm have only one stable isotope as well (see Table 1). Table 1. La 99.91

Ce

Pr 100

Nd

Isotope abundance of the rare earth series of elements Pm

Sm

Eu

Gd

Tb

Dy

Ho

100

Er

Tm

Yb

Lu

100

3. Hydrogen-Induced Low-Energy Nuclear Reactions It was a brave decision for Iwamura to select high Z material (Cs, Sr, Ba, etc.) as sample. It was also a brave decision for professor G. Miley to study the hydrogeninduced low-energy nuclear reaction. 9 In the early days, H2 was just selected as a control in comparison with D2, because most of scientists (including the members of ERAB of DOE) were thinking of the d + d fusion reaction only. Even professor M. Fleischmann was not ready to accept such new phenomena. In ICCF-7 (Vancouver, 1998), Miley asked a question during a plenary session. He would like to know what are Martin's comments on nuclear transmutation. Fleischmann

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replied with humor "I am a conventional chemist." However, the most impressive results are the four peaks in the distribution of nuclear products which appeared in various experiments in the world (Refs. 10-12). The organizer of ICCF-12 made a good program to arrange a minicourse presentation by Miley. It should be emphasized that both Miley and Iwamura used thin film samples and used super-lattice complexes in their experiments. 4. Prom DS-Cathode to DS-Reactor Professor Arata switched from electrolytic cell to gas-loading experiment while keeping his double-structure characteristics of palladium. 13 He is happy with this new structure because "Sauna-bath" is better than the "hot-water-bath." More energy output would be available from the newly designed DS-reactor. It is quite clear qualitatively to show that the temperature reverse (i.e. the temperature of heater is lower than that of the heated object) appeared when the H2 was replaced by D2, and the vacuum vessel was filled with Pd-black or Nano Pd. The most interesting point was the temperature setting. T out = 140°C was just same as that appeared in the early experiment in China, where a correlation between the deuterium flux and abnormal heat flow was found14 (Fig. 1, right-hand side).

Correlation between heat flow and deuterium

J. Phys. D: Appl. Phys. 36 (2003) 3095

Arata "Sauth bath" reactor

140°C-150°C

Figure 1. About 140°C as a characteristic temperature was discovered in both Arata's Sauna bath and an early Chinese correlation experiment where D2 gas was permeating Pd thin wall.

The DOE reviewers in 2004 asked the frequently asked questions in those excess heat experiments: "The reviewers who did not find the production of excess power convincing cite a number of issues including: excess power in the short term is not the same as net energy production over the entire of time of an experiment; all possible chemical and solid state causes of excess heat have not been investigated and eliminated as an explanation; and production of power over a period of time is

29

a few percent of the external power applied and hence calibration and systematic effects could account for the purported net effect." As a supplement to against those criticisms, we may add one more experiment: "Heat after Death" work. 15 M. Fleischmann's "Heat after Death" experiment in 1993 provided a compelling estimate. His electrolytic cell was boiled to dry in 10 min. The vaporization heat was so large (102.5 kJ) that all uncertainties in the other effects might be ignored (22.5 kJ for input from electrolysis, 6.7kJ for heat transfer to ambient). The volume of the palladium cathode was only 0.0392 cm 3 which is about 4.6 x 10~ 3 mol. Hence, the most conservative estimate would be 18.8 MJ per mol of Pd (i.e. 195 eV per Pd atom). Even if this amount of energy had have been stored in the palladium due to some unknown mechanism during the long period of electrolysis, this would have still be an anomalous "chemical" effect (if it is not a nuclear effect). Would the reviewers still say "While significant progress has been made in the sophistication of calorimeters since the review of this subject in 1989, the conclusions reached by the reviewers today are similar to those found in the 1989 review," if they had paid attention to this calculation. 5. N e w Hydrogen Energy Project and Loading Ratio Dr. Matsui kindly appeared in ICCF-12 again. His announcement about NHE project in ICCF-4 was a great impetus to Condensed Matter Nuclear Science research. At that time a program was established to aim at the high loading using electrolysis method. Adding something (e.g. thiourea, etc.) in the electrolyte was found effective to enhance the loading ratio, but the excess heat was not as great as expected. 16 The failure in helium detection and the argument on "excess heat" were partially compensated by the successful nuclear transmutation 17 and the deuterium flux effect.18 Particularly, the deuterium flux effect appeared both in the "excess heat" and in the nuclear transmutation. It turns out to be the key issue to reproduce the effects of the condensed matter nuclear science. If the 18 reviewers had have chance to review this issue, they might not be so pessimistic that "Most reviewers, including those who accepted the evidence and those who did not, stated that the effects are not repeatable,..." 6. Fundamental research in Condensed Matter Nuclear Science "... Use of reasonably well-characterized materials, exchange of materials between groups, and careful estimation of systematic and random errors" was recommended in DOE 1989 review. Then, how to characterize the material? The resistance ratio of palladium sample was widely used as an important characteristic in electrolysis and gas-loading experiment. Mckubre of SRI group, 19 and Spollane and Celani of Frascatti group 20 presented very careful measurement with close collaboration. Eight methods of measurement were summarized to relate this resistance ratio to the loading ratio of the palladium sample. It was found that the relationship between

30

resistance ratio and loading ratio was very complicated because there was no good calibration for the high loading region where the sample was supposed to work, and because the resistance depended on temperature while the temperature coefficient depended on loading ratio also. The recommendation is that resistance ratio might be still a good characteristic if we specified the temperature at which this ratio was measured. The careful study on the temperature coefficient of the resistance of the palladium hydride revealed a possible phase transition in the high loading region which might be just the region of interests for CMNS. 7. Long Life-Time State in Condensed Matter Nuclear Science Three-deuteron reaction was unexpectedly discovered while the branching ratio of the d + d fusion was measured at low energy. It was first discovered in 1993 by professor Kasagi at Tohoku University in terms of d + (d + d) —> p + n + a reaction. 21 Kasagi's experiments at low energy was very reliable that even Dr. Morrison, the famous opponent of the "cold fusion", stood up to praise Kasagi's experiments for screening effect at low energy as the best experiment in ICCF-7 (Vancouver, 1998). Indeed, professor Takahashi tried to verify this three-deuteron reaction in terms of d + (d + d) —> T + 3 He as well at Osaka University.22 This three-deuteron reaction implied that two deuterons were kept in a Long Life- Time State before two deuterons saw the third deuteron. During the ICCF-12, Kasagi proposed further the evidence of the motion of the deuteron before d + d interaction, and Takahashi proposed further the assumption of Bosonized Condensates. 23 If we look at the Bockris' paper in ICCF-11 proceedings 12 about the tritium production and the /3-decay, we may believe that this Long Life- Time State might be essential in order to understand the mechanism of the condensed matter nuclear science. If the reviewers could be aware of those facts; then, they might not say: "The studies were designed to investigate screening effects in materials that would be relevant to fields such as nuclear astrophysics. Those reviewers who commented on these studies generally viewed them favorably, but to many reviewers these studies were somewhat peripheral to the main thrust of this review." 8. Dolan's Comments and Italy—Japan Joint Projects Dr. Thomas Dolan was an officer at International Atomic Energy Agency to coordinate the fusion research in the world for United Nations (1995-2001). He was mainly working for plasma fusion projects; however, he visited some of the "cold fusion" laboratories, and even took part in the ICCF-9 (2002, Beijing) as a retired scientist. He suggested that we should establish an international society, an international journal, and an award in order to enhance the credit of our research, and break the bad cycle to obtain both the credit and the research fund. Now he attended ICCF-12 again. We have the International Society for Condensed Matter Nuclear Science, the International Journal for Condensed Matter Nuclear Science,

31

and the Preparata Medal. Professor Takahashi announced that there would be a Joint Project between Italian and Japanese scientists to explore the possibility of processing the nuclear waste using the nuclear transmutation induced by deuterium flux. The first phase would be supported by 13 million Euros and followed by second phase with 12 million Euros. 9. A Cost-Effective Study Dr. Thomas O. Passell, the Co-Chairman of the ICCF-4, proposed further his results in using discharge tube for excess heat detection. 24 He intended to use the small size gas discharge tube to make a wide-range survey on various materials for electrodes and gases while keeping the sensitivity and efficiency high enough. When the government support is still a long way to go, he used his retirement money to keep the project running. As a retired manager from the Electrical Power Research Institute, he has been optimistic towards the future of the Condensed Matter Nuclear Science. Israel group represents an excellent private company to achieve constant progress in excess heat with the best international collaboration (Mckubre of SRI, Violante of INFN). 25 DOE's recommendation, "Emphasis should be placed on calorimetry with closed systems and total gas recombination, use of alternative calorimetric methods, use of reasonably well characterized materials, exchange of materials between groups, and careful estimation of systematic and random errors. Cooperative experiments are encouraged to resolve some of the claims and counterclaims in calorimetry", has been fully realized already. 10. Prospects The situation is changing gradually towards favorable to Condensed Matter Nuclear Science. The Journal of Fusion Energy, decided to accept the submission from the Condensed Matter Nuclear Science.26 It has been mainly a hot fusion journal edited by the former DOE officer (Dr. Steve Dean), and published by the famous Springer Verlag. Springer Verlag even decided to publish an academic book about the Condensed Matter Nuclear Science as well. This "New Physical Effects in Metal Deuterides" would be disseminated eventually, and lead to a clean and sustainable energy resource for the world. Acknowledgements This work is supported by the Natural Science Foundation of China (#10475045), Ministry of Science and Technology (Division of Fundamental Research), and Tsinghua University (985-11, Basic Research Funds). I would like address that we are grateful to Professor A. Takahashi, Dr. Y. Iwamura, Professor K. Ota, and the local organization committee for a very successful ICCF-12. It was well planned, well organized and well programmed.

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References 1. Cold Fusion Research, DOE/S-0073, A report of the energy research advisory board to the united states department of energy (1989). 2. Peter L. Hagelstein, Michael C.H. McKubre, David J. Nagel, Talbot A. Chubb, and Randall J. Hekman, New Phys. Eff. Met. Deuterides (2004). 3. U.S. Department of Energy Cold Fusion Review Reviewer Comments, http://www. newenergytimes.com/DOE/DOE.htm (2004). 4. Y. Iwamura et al., Observation of surface distribution of products by X-ray fluorescence spectrometry during D2 gas permeation through Pd complexes, Presentation ICCF-12, Yokohama, Japan, November 27-December 2 (2005). 5. T. Higashiyama, A. Takahashi et al., Replication of MHI transmutation experiment by D2 gas permeation through Pd complex, in: P. Hagelstein, S.R. Chubb (eds), World Scientific (New Jersey, 2006), Proc. ICCF-10, Cambridge, USA, 24-29 August (2003). 6. S. Narita et al., Discharge experiment using P d / C a o / P d multi-layered cathode, Presentation ICCF-12, Yokohama, Japan, November 27-December 2 (2005). 7. H. Yamada et al., Producing transmutation element on multi-layered Pd sample by deuterium permeation, Presentation ICCF-12, Yokohama, Japan, November 27December 2 (2005). 8. G.S. Qiao, X.Z. Li et al., Nuclear products in a gas-loading D/Pd and H/Pd system, Proc. ICCF7, Vancouver, Canada, April 19-24, ENECO, Inc., Salt Lake City, UT (1998). 9. G.H. Miley, Overview of light water/hydrogen-based low energy nuclear reactions, Presentation ICCF-12, Yokohama, Japan, November 27-December 2 (2005). 10. T. Mizuno, T. Ohmori and M. Enyo, Change of isotope distribution deposited on palladium induced by electrochemical reaction, J. New Energy 1(1), 23 (1996). 11. T. Ohmori and M. Enyo, Iron formation in gold and palladium cathodes, J. New Energy 1(1), 15 (1996). 12. J.O-M. Bockris, Histroy of the discovery of transmutation at texas A & M university, in: Jean-Paul Biberian (ed.), World Scientific (New Jersey 2006) Proc. ICCF-11, Marseilles, France, 31 October-5 November (2004), p. 562. 13. Y. Arata and M.J.A.Y.C. Zhang, Development of 'DS-Reactor' as the practical reactor of cold fusion based on the 'DS-CelF with the 'DS-Cathode', Presentation ICCF-12, Yokohama, Japan, November 27-December 2 (2005). 14. X.Z. Li, Jian Tian et al., Correlation between abnormal deuterium flux and heat flow in a D/Pd system, J. Phys. D: Appl. Phys. 36, 3095 (2003). 15. M. Fleischmann and S. Pons, Calorimetry of the Pd-D20 system: from simplicity via complications to simplicity, Phys. Lett. A 176, 118 (1993). 16. A. Kubato et al., Development and experiments on a flow calorimetry system, in: M. Okamoto (ed.), Proc ICCF-6, Toya, Japan, 13-18 October (1996), Vol. 1, p. 52. 17. G.H. Miley et al, Quantitative observation of transmutation products occurring in thin-film coated microspheres during electrolysis, in: M. Okamoto (ed.), Proc ICCF6, Toya, Japan, 13-18 October (1996), Vol. 2, p. 629. 18. Y. Iwamura et al., Correlation between behavior of deuterium in palladium and occurrence of nuclear reactions observed by simultaneous measurement of excess heat and nuclear products, in: M. Okamoto (ed.), Proc. ICCF-6, Toya, Japan, 13-18 October (1996), Vol. 1, p. 274. 19. M.C.H. Mckubre et al., Using resistivity to measure H/Pd and D/Pd loading: method and significance, Presentation ICCF-12, Yokohama, Japan, November 27-December 2 (2005).

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20. A. Spallone, F. Celani et al, Measurements of the temperature coefficient of electric resistivity of hydrogen overloaded Pd, Presentation ICCF-12, Yokohama, Japan Novembew 27-December 2 (2005). 21. J. Kasagi et al., Energetic protons and alpha particles emitted in 150-keV deuteron bombardment on deuterated Ti, J. Phys. Soc. Jpn 64(3), 777 (1995). 22. A. Takahashi et al, Studies on 3D fusion reactions in TiDx under Ion beam implantation, in: P. Hagelstein, S.R. Chubb (eds), World Scientific (New Jersey, 2006), Proc. ICCF-10, Cambridge, USA, 24-29 August (2003) p. 657. 23. A. Takahashi, Time-dependent EQPET analysis of TSC, Presentation ICCF-12, Yokohama, Japan, November 27-December 2 (2005). 24. T.B. Benson and T.O. Passell, Glow discharge calorimetry, Presentation ICCF-12, Yokohama, Japan, November 27-December 2 (2005). 25. I. Dardik et al., Progress in electrolysis experiments at energetics technologies, Presentation ICCF-12, Yokohama, Japan, November 27-December 2, (2005). 26. X.Z. Li et al., A Chinese view on summary of condensed matter nuclear science, J. Fusion Energy 23(3), 217 (2004).

OVERVIEW OF LIGHT W A T E R / H Y D R O G E N - B A S E D LOW E N E R G Y N U C L E A R REACTIONS

G E O R G E H. M I L E Y Department

of Nuclear, Plasma and Radiological Engineering, 103 S. Goodwin Avenue, Urbana, IL 61801, E-mail: [email protected]

University USA

of

Illinois,

P R A J A K T I J. S H R E S T H A NPL Associates

Inc.,

912 W. Armory Avenue, Champaign, E-mail: [email protected]

IL 61821,

USA

This paper reviews light water and hydrogen-based low-energy nuclear reactions (LENRs) including the different methodologies used to study these reactions and the results obtained. Reports of excess heat production, transmutation reactions, and nuclear radiation emission are cited. An aim of this review is to present a summary of the present status of light water LENR research and provide some insight into where this research is heading.

1. Introduction This review focuses on the transmutation reactions and excess heat production in experiments using light water electrolysis or hydrogen gas/plasma loading undergoing low-energy nuclear reactions (LENRs). Although most LENR ("cold fusion") research has focused on heavy water, a considerable number of experiments have used light water electrolysis or hydrogen gas loading. A few experiments have attempted to compare the results from light versus heavy water, 1 - 4 but these comparisons remain inconclusive. There are a wide variety of cold fusion nuclear reactions. As shown in Fig. 1, the original Pons-Fleishmann (P-F) reaction involved DD fusion, where unlike in hot fusion, the reaction channel is "interrupted" through deactivation of the excited He4 reaction product by energy transfer to the host lattice, ultimately heating the lattice. Alternately, a number of researchers have reported transmutation reactions that involve interactions between deuterium (or hydrogen) directly with atoms in the host lattice, typically heavy metals. This branch of "cold fusion" is commonly termed LENR, although recently there has been a move to also term P - F type DD reactions as LENRs as well. The observation of nuclear reactions between electrolyte and host metal atoms is quite unexpected due to the very large coulombic barrier involved (much larger than for D-D reactions). Consequently, one purpose of this review is to bring together much of the data accumulated on this striking new phenomenon. The readers are 34

35

left to decide for themselves if the data is adequate to establish the case for such reactions and possibly to formulate new experiments that build on and extend this data base. About 40 publications were included in this review (see references herein). This was intended to be representative but not exhaustive of the field. Researchers wishing to add information to the data base are invited to contact the authors. D-D Reactions T +p

% branching hot fusion "P—F" type 50 < 0.1

D - D - > He-3+ n

50

He-4 + gamma

< 10

< 106 99+

LENRs p + metal —fc- products or "fission" product array Figure 1. Comparison of LENR reactions and DD reactions occurring in hot and "cold" ( P - F type) fusion.

1.1.

Methodology

A summary of various methods employed for this study is given in Table 1. A majority of the researchers cited used electrolysis to study LENR: Pd/Pt, Ni/Pt were commonly used electrodes. K2CO3 is a popular choice as an electrolyte, a trend perhaps started by the Mills and Kneizy's early experiments where extremely large reaction rates were reported. Gas loading is also frequently used while a few researchers have reported using a glow discharge (GD) plasma. 1.2. Early Studies

at

UIUC

Earlier work by one of the authors (Miley) in collaboration with Patterson represents one of the more extensive studies of light water electrolysis relative to reaction products and excess heat. About 1000 microspheres (~0.5cm 3 volume) were used in a packed-bed electrolysis cell. Thin films of Ni and/or Pd were coated on the beads to serve as the cathode. The electrolyte was 1 M Li2S04 light water electrolyte with a flow rate of ^ l l m l / m i n through the packed bed. Voltages across the bed were held at ~2-3 V, with several mA of current, giving an electrical input power of approx. 0.06 W. Significant excess heat and a fission-like reaction product array were reported. A detailed description of the experiment can be found in Ref. 1. 1.3. Reaction

Product

Analysis

Method

Reaction products have been analyzed using a variety of precision mass analysis techniques. For example, Miley et al. used a combination of NAA, SIMS, Energy Dispersive X-ray (EDX) analysis and Auger Electron Spectroscopy (AES). 1 Cirillo

36 Table 1. Summary of various methods employed for light water/H2 LENR studies (data collected for this and following tables and figures use Refs. 1—35) Electrolysis

Total

Electrode Pt/Pd Pt/Ni Pt/W Pt/Au Pt/Sn Pt/Re Pt/Ti Pt/Ag Pt/Pt

14 5 3 4 1 1 2 1 2

Electrolyte K2CO3 H2SO4 Na2C03 Li2S04 KOH Na2S04 CS2SO4 H20

10 3 5 4 1 5 1 2

GD plasma Gas loading

1 5

and Iorio used SEM to study transmutation products. 9 Arapi et al. used TOFSIMS for product analysis. 5 Iwamura et al. used XPS extensively in their studies, although they concentrated on D2 gas experiments (versus H2), so are not included in this survey per se. 36 2. Results 2.1. Transmutation

Products

A quantitative measure of the yield of transmutation products (and isotopic shifts from natural distribution in key products) in four major atomic groups (6-18, 22-35, 44-54, and 75-85) were obtained by Miley et al.1 Others also have reported significant nuclear reaction products and isotopic shifts in light water LENRs. In some cases of the observed elements were from the lanthanide group, including Lu, Tb, Pr, Eu, Sm, Gd, Dy, Ho, Nd, and Yb. It is widely accepted that these rare earth elements are less likely to be found as impurities, strengthening confidence in their results (although most researchers have tried to rule out mistakes due to impurities versus the common "product" elements such as Fe, Cu, Ag, Zn, Au, etc via analysis of cell components, electrodes and electrolyte prior to LENR runs).

37

Isotopic shifts are another key feature often cited against mistaken identification of impurities as reaction products. Violante's study showed that the 6 3 Cu/ 6 5 Cu isotopic ratio shifted.33 In this Ni-hydride film work the most abundant copper isotope was 65 Cu with a shift from natural distribution by f360%. Cirillo and Iorio found Re, Os, Au, Hf, Tl, Er, and Yb on the surface of the cathode, which was not present before the reactions. 9 Ohmori et al. reported finding Hg, Kr, Ni, and Fe with anomalous compositions in Au electrodes during light water electrolysis.29 In addition Si, Mg with other anomalous compositions were also detected in the precipitates separated from the Au electrode after electrolysis at extremely high current densities. They found significant deviations from natural values. Minor product elements such as Os, W, and Ru in particular showed large deviation, whereas elements with larger yields like Pb and Ag rarely showed significant deviations. Yamada et al. also reported a large increase of Cr, Fe, Cu, and Ag in their experiment where Pd was loaded with hydrogen gas. 35 Arapi et al. found Be and Ni in heavy water while in light water LENR they report Li, Ba, and Ni. 5 Dash et al. reported formation of Au and Ag in both light and heavy water LENR; however, the concentrations were somewhat higher in the heavy water experiments. 10 Table 2 summarizes the list of elements observed in light water by the number of times they were reported being produced in their research by different research groups. Fe and Cu were commonly observed. Rare earth elements were reported less frequently. Also note that a majority of the transmutated elements reported have changes in their isotopic composition from the natural abundance. It is interesting that the frequency of observation of light water LENR elements is not significantly different from heavy water LENR (for the latter see Ref. 37). Table 2. The total numbers of reports that state the elements were produced in their experiment Observation frequencies

Transmutation elements

1 2 3 4 5 6 7 8 11

As, Ge, S, Hg, Kr Cd, Rr , Au, Hf, Th, Er, Yb, B, V, Cs Li, Ba, Al, Os, C, Si Mg, Mn, Co, P b Ag, CI, Ti Ni, K Ca, Cr, Zn Cu Fe

One way to evaluate this data is to consider a confidence level of >6 observations. Then Ni, K, Ca, Cr, In, Cu, and Fe meet the criteria (Fig. 2). However, it can be argued that the potential impurity levels for some of the less frequently observed elements are very low, raising the signal/noise confidence level for those observations despite their less frequent observation.

38

Figure 2. This graph shows the frequency of observation for various transmutated elements designated by atomic number.

2.2. Radiation

Emission

Recent experiments using various methods of loading hydrogen have shown significant soft X-ray emission in certain specialized experiments, e.g. see Ref. 38. Also MeV energy charged particles have been reported. Alpha particles and protons have been identified with energies around 11.0-16.0 and 1.7 MeV, respectively. During electrolysis of thin Pd-film cathodes on dielectric substrates as well as from Pd-black electrode surfaces. Only very weak X-ray emission was found in these experiments, the upper dose limit (corresponding to 4, Pd/Ni electrode electrolysis experiment, which is more than 5% excess. 14 However, this excess heat was always reproducible. It is not conclusive whether using light water or heavy water produces more excess heat. Some research has reported that heavy water produced relatively larger excess heat and more transmutation products, 7 ' 1 0 while some have indicated that in both cases the excess heat and reaction products were similar. 31 Direct comparison is complicated since many parameters are modified with an electrolyte substitution. Thus, much work is required before carrying out a meaningful comparison. The excess energy for light water/H 2 LENR reported by various researchers tends to be either low (25%), with few reports of intermediate values (see Table 3, Fig. 3). More quantitative analysis is required to understand if this "two tier" result has a basic cause. Table 3. The range of excess energy various reports have achieved in their experiment Excess energy (%) 0-5 6-10 11-15 16-20 21-25 26-30 31-35 35+

2.4. Historical

Number reported 2 2 0 0 1 3 0 2

Trends

A review of historical trends indicates that a majority of researchers have examined both the transmutation reactions and excess heat generation, strongly suggesting that they expect both phenomenon in light water LENR. However, considerable work has also continued to study these phenomenons separately. Table 4 shows that heavy activity occurred in the early 1990 period, and then decreased. However, starting in 2000 onward, research in light water LENR again increased in activity.

40

Excess energy (%) Figure 3.

This graph shows Table 3 data in a graphical presentation.

This suggests that some time was required for researchers to digest the early work and become interested in devoting time to this new area of LENR.

3. Theory Many different theories have been proposed for the mechanism of reactions that takes place in LENR. However, a definitive match of theory and experiment has yet to be achieved. Thus the "best" theory remains unclear. In order to explain how the large Coulombic barrier is overcome, many theories introduce a neutral particle in the reaction matrix. Some of the theories of this type include Neutron Cluster formation by Fisher, 40 Free Neutron Reactions by Kozima, 41 R-Matrix Theory by Chubb, 42 Shrunken Hydrogen by Mills,43 Electron-Proton capture by Stoppini 44 and Proton/Deuteron Cluster by Dufour.45 The challenge now is to sort out how any of these theories can explain the unique signatures of heat and varied transmutation products reported experimentally.

Table 4.

Survey of the year and the key signatures of LENR focused in the study Years

Type of study Excess head and transmutation Excess head studies — transmutation not studied Transmutation studies — excess head not studied Excess head studies - transmutation not found

1990-1994 4 6

1995-1999 2 1 3

2000-2005

Total

6 1 5 1 Total

12 8 8 1 29

41 4.

Conclusions

In view of the rather extensive d a t a base for light water/hydrogen-based LENR, it is rather convincing t h a t this phenomenon is real. Since the measurements are very tedious and demanding, some errors are no doubt contained throughout the database. (The authors did not feel qualified to rule out any seriously reported d a t a by competent researchers.) However, it seems highly unlikely t h a t all of the d a t a are erroneous. From a practical point of view, the issue remains whether or not there is any unique advantage of light water/hydrogen L E N R versus heavy wat e r / d e u t e r o n LENR. Two applications are at issue for both: heat production a n d / o r transmutation. However, the experiments surveyed here suggest t h a t at this stage there is no clear evidence whether or not heavy water is more favorable t h a n light water for either application. Clearly many more comparative studies are essential t o clarify this issue. Another aspect is t h a t the heat reaction in these two cases appears to produce different reaction products. Thus, for wide applications involving public exposure the reaction products need t o be carefully evaluated relative to environmental compatibility a n d radioactivity. This evaluation not only applies t o the main reaction but possible parasitic ("side") reactions.

Acknowledgments We would like to t h a n k all the researchers in the field who has provided significant contribution in preparation of this paper. This work was partially supported by a grant from the New York Community Trust.

References 1. G.H. Miley, G. Name, M.J. Williams, J.A. Patterson, J. Nix, D. Cravens, and H. Hora, Prog. New Hydrogen Energy 2, 629 (1997). 2. J. Dash, G. Noble, and D. Diman, Trans. Fusion Technol. 24, 299 (1994). 3. J. Dash, G. Noble, and D. Diman, Surface Morphology and Microcomposition of Palladium Cathodes After Electrolysis in Acidified Light and Heavy Water: Correlation With Excess Heat, ICCF 4, Lahaina, Maui (1994). 4. J. Dufour, J. Foos, J.P. Millot, and X. Dufour, Fusion Technol. 31 198 (1997). 5. A. Arapi, R. Ito, N. Sato, M. Itagaki, S. Narita, and H. Yamada, Experimental observation of the new elements production in the deuterated and/or hydride palladium electrodes, exposed to low energy DC glow discharge, ICCF-9, Tsinghua Univ., Beijing, China, May 19-24 (2002). 6. R.T. Bush, Fusion Technol. 22, 301 (1992). 7. C.S. Cano, Comparison of Heat Output and Microchemical Changes of Palladium Cathodes under Electrolysis in Acidified Light and Heavy Water, MS Thesis, Portland State University (2002). 8. C.H. Castano, A.G. Lipson, S.O. Kim, and G.H. Miley, Calorimetric Measurements during Pd-Ni thin film-cathodes Electrolysis in L12SO4/H2O Solution, Proc. ICCF-9, Beijing, China, pp. 24-28, May 19-24 (2002). 9. D. Cirillo and V. lorio, Transmutation of metal at low energy in a confined plasma in water, ICCF11, Marseille, France (2004).

42

10. J. Dash and G. Noble, Intern'l. Symp. On Cold Fusion and Advanced Energy Sources, Belarusian State University, Minsk, Belarus, May 24-26 (1994a). 11. J. Dash and D. Chicea, Changes In The Radioactivity, Topography, And Surface Composition Of Uranium After Hydrogen Loading By Aqueous Electrolysis, ICCF-10, Cambridge, MA (2003). 12. M. Di Giulio, E. Filipppo, D. Manno, and V. Nassisi, Intrn'l J. Hydrogen Energy 27, 527 (2002). 13. J. Dufour, J. Foos, and J.P. Millot. Measurement of Excess Energy and Isotope Formation in the Palladium-Hydrogen System, ICCF-5, Monte-Carlo, Monaco: IMRA Europe, Sophia Antipolis Cedex, France (1995). 14. M. Fujii, S. Mitsushima, N. Kamiya, and K.Ota, Heat measurement during light water electrolysis using Pd/Ni rod cathodes, ICCF9, Beijing, China, May 19-24 (2002). 15. T. Hanawa, Z-ray Spectrometric Analysis of Carbon Arc products in Water, Proc. ICCF-8, Italy, 147 (2000). 16. X.Z. Li, Y. Deng, Y.J. Yan, H.F. Huang, W.Z. Yu, and C.X. Li, J. New Energy 6, 1, 80 (2001). 17. G.H. Miley, Product characteristics and energetics in Thin-Film electrolysis experiments, Proc. ICCF-7, Vancouver, Canada, 241, April 19-24 (1998). 18. R.L. Mills and S.P. Kneizys, Fusion Technol. 20, 65 (1991). 19. R. Mills, M. Nansteel, and P. Ray, J. Plasma Phys. 69, 131 (2003). 20. R. Mills, J. He, Z. Chang, H. Zea, K. Akhtar, Y. Lu, C. Jiang, and B. Dhandapani, Catalysis of Atomic Hydrogen to Novel Hydrides as a n New Power Source, 230 ACS National Meeting, Washington DC, Aug 28-Sept 1 (2005). 21. D.W. Mo, Q.S. Cai, L.M. Wang, and X.Z. Li, The Confirmation of Nuclear Transmutation Phenomenon in a Gas Loading H/Pd System Using NAA, ICCF-7, Vancouver, Canada, 105, April 19-24 (1998) 22. T. Mizuno, T. Ohmori, and A. Akimoto, Generation of Heat and Products During Plasma Electrolysis, ICCF-10 (2003). 23. V. Noninski, Fusion Technol. 2 1 , 163 (1992). 24. R. Notoya, Y. Noya, and T. Ohnishi, Fusion Technol. 26, 179 (1992). 25. R. Notoya, Nuclear Products of cold Fusion Caused by Electrolysis in Alkali Metallic Ions Solutions, Proc. ICCF-5, Monte-Carlo, Monaco, pp.531-538, April 9-13 (1995). 26. T. Ohmori and M. Enyo, Fusion Technol. 24, 293 (1993). 27. T. Ohmori and M. Enyo, J. New Energy 1, 15 (1996). 28. T. Ohmori and T. Mizuno, Observation of the Product Elements of Nuclear Transmutation Reaction on/in Several Metal Electrodes by the Cathodic Electrolysis in Light Water Solutions, ICCF-7, Vancouver, Canada, p. 109, April 19-24 (1998a). 29. T. Ohmori, T. Mizuno, Y. Nodasaka, and M. Enyo Fusion Technol. 33, 367 (1998). 30. T. Ohmori and T. Mizuno, Strong Excess Energy Evolution, New Elements Production, and Electromagnetic Wave and/or Neutron Emission in the Light Water Electrolysis with a Tungsten Cathode, Proc. ICCF-7, Vancouver, Canada, 279 (2000). 31. T. Ohmori, H. Yamada, S. Narita, and T. Mizuno, Excess Energy and Anomalous Concentration of K Isotopes in Potassium formed on/in a Re Electrode during the Plasma Electrolysis in K 2 C 0 3 / H 2 0 and K 2 C 0 3 / D 2 0 Solutions, Proc. ICCf-9, 284, May 19-24 (2002). 32. T. Ohmori and M. Enyo, Fusion Technol. 24, 293 (1993). 33. V. Violante, E. Castagna, C. Sibilia, S. Paoloni, and F. Sarto, Analysis Of NiHydride Thin Film After Surface Plasmons Generation By Laser Technique, ICCF 10 (2003).

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34. H. Yamada, S. Narita, Y. Fujii, T. Sato, S. Sasaki, and T. Ohmori, Production of Ba and several Anomalous Elements in Pd under light Water Electrolysis, ICCF-9, Beijing, China, 123, May 19-24 (2002). 35. H. Yamada, S. Narita, H. Onodera, H. Suzuki, N. Tanaka, T. Nyui, and T. Ushirozawa, Analysis By Time-Of-Flight Secondary Ion Mass Spectroscopy For Nuclear Products In Hydrogen Penetration Through Palladium, ICCF10 (2003). 36. Y. Iwamura, T. Itoh, M. Sakano, N. Yamazaki, S. Kuribayashi, Y. Terada, T. Ishikawa, and J. Kasagi, Observation of Low Energy Nuclear Reactions Induced By D2 Gas Permeation Through Pd Complexes, ICCF- 9, Beijing, China (2002). 37. G.H. Miley and P.J. Shrestha, Review of Transmutation Reactions in Solids, Proc. ICCF 10, Cambridge, MA, Aug 24-29 (2003). 38. G.H. Miley, P.J. Shrestha, and H. Hora, Current Trends in International Nuclear Research, (Ed.) E. Panarella, NRC Research Press, Ottawa, Canada (2003). 39. A.G. Lipson, A.B. Karabut, and A.S. Roussetsky, Anomalous enhancement of DDreaction, alpha emission and X-ray generation in the high current pulsing deuterium glow-discharge with Ti-cathode at the voltages ranging from 0.8-2.5 kV, ICCF-9, Beijing, China, (2002). 40. J.C. Fisher, Theory of Low-Temperature Particle Showers, ICCF-10, (2003). 41. H. Kozima, CF-Matter and the Cold Fusion Phenomenon, ICCF-10, (2003). 42. S.R. Chubb, Framework for Understanding LENR Processes, Using Conventional Condensed Matter Physics, ICCF-11, Marseille, France, (2004). 43. Black Light Power Inc. Website, accessed on 11/10/2005, http://www.blacklightpower.com/ techpapers.shtml. 44. G. Stoppini, Fusion Technol. 34, 81 (1998). 45. J. Dufour, J.H. Foos, and X.J.C. Dufour, Infinite Energy 4, 53 (1998).

DEVELOPMENT OF "DS-REACTOR" AS THE PRACTICAL REACTOR OF "COLD FUSION" BASED ON THE "DS-CELL" WITH "DS-CATHODE"

YOSHIAKI ARATA AND YUE-CHANG ZHANG Center for Advanced Science and Innovation, Osaka University, 2-1 Yamadaoka, Suita, Osaka 667-0871, Japan E-mail: arata@casi. osaka-u. ac.jp

It is well known that Double Structure Cathode ("DS-cathode") presented exactly evidence of strong cold fusion reaction, but could not use as the Practical Reactor because the most of the input energy is consumed inside the electrolyte as the energy loss; it means the "bad-efficiency". Then, to get "good-efficiency", we proposed a new "DS-cell" without the electrolyte, and named as the "DS-reactor" for this new DS-Cell to be utilized as the practical reactor. Therefore, it was concluded that DS-reactor adopted D2 gases with low temperature such as 100-200° C and suitable pressure of about 1—100 atm instead of D2 0-electrolyte as the nuclear fuel, and DS-reactor is constructed with following double structure, for instance, outer stainless-vessel and inner Pd-vessel. Moreover, DS-reactor is classified into two kinds of A-type and B-type based on the combination of between (sample and D2 gas) and (stainless-vessel and Pd-vessel); that is, A-type is combined to keep D2 gas inside outer vessel and sample inside Pd vessel with high vacuum condition and B-type is combination of D2 gas inside Pd-vessel and sample inside outer vessel. In this case, selection of the sample is the most important and should be adopted the sample to produce innumerable "Pycnodeuterium" inside the sample. Using the DS-reactor, existence of Cold Fusion was verified with "good-efficiency" to be utilized as the practical reactor.

1. Introduction In order to understand the function of the Double Structure Reactor (DS-reactor), it is important to know the principle of DS-cell/DS-cathode. 1 DS-cell is constructed with electrolyte ( D 2 0 / H 2 0 + LiOH) and DS-cathode together with Pt-cylindrical anode, and structure of DS-cathode is constructed with closed Pd-cylinder in which sample (nano Pd/Zr3NiO/Pd black, ...) is kept inside ultrahigh vacuum hollow space. When DS-cell is electrolyzed, the vacuum hollow space is filled up easily with ultrahigh pressure gas (D 2 /H 2 : 10 3 -10 4 atm) and the innumerable solid "Pycnodeuteriums" are produced inside the Sample.2 We discovered that the "Pycnodeuterium" cause easily nuclear reaction ("cold fusion") using not only DScell but also laser welding solid fusion reactor, sonoimplantation solid fusion reactor, 44

45

which were invented by us. However, these devices gave "bad efficiency; that is, their input energy was too large. Figure f shows principle of "DS-cell" and it will be given intuitive understanding for the principle. 3

© t

ID

12-



Samples enclosed inside high vaccum Pd vessel

This white space becomes ultrahigh pressure Ds gas (~104 atm) in this patent

DS-cathode/DS cell for cold fusion

Figure 1.

Illustrated principle of "DS-cathode"/ "DS-cell"

Note: This is US-patent, 3 method of producing ultrahigh pressure; and it is realized by extremely pure deuterium with ultra-high over 10 000 atm pressure using electrolytic method. Fifty years ago, in 1955-1958, for the first time in Japan, we opened to the public the thermonuclear fusion experiment caused by generating several million centigrade degree with a current of several million ampere, which were the highest current and temperature in the world at that time. But Japanese could not buy deuterium gas in the market place at that time. Then, we generated deuterium gas by the same system of this device, which were made by oneself. This event was described in a US-magazine of the 21st century science and technology in detail. 4 Then, we thought this device will be used for cold fusion and named it "DScathode" / "DS-cell", then it can be easily understood intuitively relation between this US patent and "DS-cathode" / "DS-cell" from this figure. This situation was very important.

46

2. Graphic Illustration for "DS-Reactor" As already mentioned above, we had an idea that most of the input energy was consumed inside the electrolyte as energy loss, we proposed a new concept, which is a new DS-cell with no electrolyte. We call this new type DS-cell with no electrolyte as "DS-reactor". However, the principle is the same as shown in Fig. 2. "DSreactor" exhibited good results as we expected.

Q DS-cathode (Pd-olosed cylinder) © Anode (Pt-cylinder)

Heater

Heater

Pd vessel • Stainless steel vessel

DS-reactor Figure 2. "DS-reactor" was developed based on the "DS-cell", that is, the same principle in both methods. "DS-reactor" corresponds to "DS-cell" without electrolyte, and it is considered that "DS-reactor" includes A- and B-systems.

47

Two types of "DS-reactors" as shown in Fig. 2 are invented from "DS-cell". Upper side of the figure shows the usual "DS-cell" and the lower side diagrams describe A-type (left-hand side) and B-type (right-hand side) of "DS-reactors". Both "DS-reactors" are constructed with stainless vessel as outer vessel and Pd vessel as inner vessel as shown in the lower side of the diagram. D2/H2 gas is supplied to the gray zone space with high-vacuum conditions as indicated in A-type/B-type DS-reactors and kept to pressure, P atm, and temperature, T°C, that is (Pout, Tout) in A-type reactor and (P; n , Tin) in B-type reactor. Samples are set inside the white color zone space in both reactors, and after that, the samples and white space are kept in high-vacuum condition with the same condition in white zone of DS-cell (upper-side of the diagram).

Condition

(

No sample + D2

)

Pd vessel •

^

Sample: no sample 05/10/11-12 (purs Dj) Heat-Current \

•o

3

120 180 240 300 360 420 480 540 600 660 720

60 120 180 240 300 360 420 480 540 600 660 720

Time (min) Figure 3.

Time (min)

Characteristics of "DS-reactor" without sample during D2 gas charge.

Recently, we performed four kinds of experiments using the A-type "DS-reactor", and changed experimental conditions by setting different samples inside the inner vessel with white zone and different gases inside the outer vessel with gray zone. 3. Experiment 3.1. "Experiment-1"

([A]: No Sample + D2)

Figure 3 shows the results in the first set of the experiment. ("Experiment 1", [A]). In this case, inside the Pd vessel (white zone) is vacant (no sample) and D2 gas

48

filling up with 40 atm as the outside pressure (P ou t) of Pd vessel (gray zone) as the set-conditions before the experiment. When D 2 gas under P o u t of 40 atm is heated to 140°C as the giving temperature (Tout = 140°C), Pd vessel is heated by such D 2 gas accordingly, temperature of Pd vessel never goes higher temperature than the D 2 gas. When Pd vessel reaches to 70-100°C, D 2 molecules passing through the wall of Pd vessel as D + and enter inside the Pd vessel as D atom and becomes to mixed gas [D + D 2 (= D + D)] as time passes. As a final result, inner temperature of Pd vessel (white zone), T;n, never exceed the outer temperature as the giving temperature of the D 2 gas (gray zone), T o u t , that is always T out > T-m. These results were exactly confirmed by the experiment shown in Fig. 3, Namely, experimental results of left side AQ in Fig. 3 indicates the relation between D 2 gas pressure (P ou t = 40 atm) and temperature (T out = 140°C), which were supplied into the outside Pd-vessel (gray zone) and the penetrated inner D(D 2 ) gas pressure {P-m) and temperature (Tin) inside the Pd vessel (white zone), In other words, ( P n , T in ) never exceeds (P ou t, T o u t ): always P i n < P o u t and T in < T o u t . On the right-hand side Ai, only the scale of the temperature axis of Ao shown on left-hand side is enlarged to give distinct difference between Tout and T-m.

120 180 240 300 360 420 480 540 600 660 720

Time (min) Figure 4.

0

60 120 180 240 300 360 420 480 540 600 660 720 7

Time (min)

Comparison between figures A and B (Ai is the same with Ai in Fig. 3).

49

3.2. "Experiment-2"

([B]: Sample-)- H2) (Pd

black)

Bottom-right side diagram (Fig. 4, Bi) is the experimental result of the second set-condition (Experiment 2; [B]) with sample Pd black + H 2 . This means Pd black is set as a sample inside the Pd vessel (white zone) and kept under high-vacuum condition, and H2 gas with 40 atm is filled up as the outside pressure (P0ut) of the Pd vessel (gray zone) as the set-conditions before experiment. The experiment was performed under the same process of (Experiment 1, [A]). When H 2 gas is given with P ou t of 40 atm and Tout of 140°C inside the gray zone, H atoms penetrated into the Pd vessel are absorbed inside the Pd black, and the temperature difference T as Tout-Tin becomes a little smaller than that in (Experiment1; [A]) as shown in the relation between data Ai and Bi in the bottom side diagram (A and B in Fig. 4); here, both Ai in Figs. 3 and 4 are the same diagram. As a result, inner temperature Xin was always lower than given temperature -*- out; -^ out ^ -^ in-

And both temperatures were never reversed. This result is extremely important. We have expected that nano Pd is far better than Pd black as a sample because 1,2 we have obtained that nano Pd generated excess heat with much higher rate than

D (

Sample: nano Pd + D2

Sample: Pd black; gas: D; " \ W N —

141

• : Sample: Pd black » 05/10/11-12 (pure D2)

/"in

ff

140 139

/ Heat-Current \ \ stop )

'out

-0 Pout

13R

^

™

137

.

^^--^

?

Tl

: tem

2. Q-

sure

Pi

134

^3

CO

136

hf

TO

CD

=s

m

135

O ?

a -! '

h-°

v

133

,-

h~

132 131

/ 0

60 120 180 240 300 360 420 480 540 600 660 720 780 840

Time (min)

Figure 5.

) 120180 240 300 360 420 480 540 600 660 720 780 840

Time (min)

Comparison between figures C and D.

50

that of Pd black using "DS-cell" with "DS-cathode". Experimented data can be compared with Di in ("Experiment 4", [D]) and Ci in (Experiment 3, [C]) and T;n* becomes considerable higher than T o u t in case of Di experiment against Ci experiment as shown in Fig. 5. Moreover, T;n* in Di pulled up even the first giving temperature (T out ) of 140°C to over 180°C. It is concluded that "DS-reactor" will be workable as a "practical reactor".

3.3. "Experiment-3"([C]: sample "Experiment 4"([D]: sample

(Pd black) + D2) and (nano-Pd) + D2)

Figure 5(C) in the bottom-side shows the experimental result of the third setcondition: (Experiment 3; [C]), with sample Pd black + D 2 . This means D 2 gas is used instead of H 2 gas under the same condition as (Experiment 2, [B]). As a result, wonderful phenomena were produced that temperature inside Pd vessel (T n *) becomes higher than the giving temperature, T o u t , when the D 2 gas was supplied into the gray zone (outside of Pd vessel), that is T;n* > T o u t . Experiment's data can be compared with Ci in Fig. 5 and Bi in Fig. 4. That is, compared with the functions of H 2 gas and D 2 gas which induced "temperature inversion'" inside the Pd vessel (white zone) against the giving temperature (T out ) when the D 2 gas was supplied to outside Pd vessel (gray zone). This result clearly means generation of "pycnodeuterium nuclear reaction" inside Pd vessel (white zone). Figure 5(D) shows the experimental results of the forth-set condition ("Experiment 4", [D]) with sample of "nano Pd"+D 2 . We have already reported that D2/H2 gas can be much more absorbed inside nano Pd than Pd black and innumerable "pycnodeutrium" can be produced inside nano Pd. 1 ' 2

3.4. Fundamental

Characteristics

Between

(T-m, TOVLt) and (P-m,

Pout)

Figure 6 shows the summary of the experimental data of the temperatures and the pressures demonstrated through the (Experiments 1-4). In the case of without D 2 or without the sample such as Pd fine powder, Tin never went higher than the given temperature T o u t . On the other hand, when the samples produced "pycnodeuterium", T n was always higher than T ou t, that is, caused the temperature inversion. It is also noted that the degree of this excess of temperature depends on the type of the host material; that is whether the host materials can absorb much pycnodeuterium or not. In other words, "DS-reactor" certainly displayed the similar basic characteristics of the "DS-cell", but it gave the excellent characteristics as the fusion reactor much more clearly.

51

Summary of experimental data

0£>0iM

TV. ( Sample+D 2 ) Dependence on samples Nuclear fission zone ) No sample + D2 Sample + H2

Sample

Figure 6. Illustration of fundamental characteristics between gaseous temperature (T; n , T o u t) and pressure (Pi n , Pout) in "DS-reactor".

4. Conclusion Figure 7 shows the conclusion of the experiments already described, and demonstrates the present situation of "DS-reactor" as the practical reactor of "coldfusion". From the left-hand side of the horizontal line, the thick black and thin black dots correspond to Experiments 1-4. The vertical axis represents the T;n, which is inner temperature in the gray zone of the DS-reactor. For Experiments 1 and 2, Tjn's are lower than T o u t , that is, the efficiencies are always negative. For Experiments 3 and 4, T in *'s are higher than the given temperature T o u t . This means that these efficiencies were always positive and moreover, almost of the input energy was collectable. It is emphasized that T;n for Experiments 1 and 2 are always lower than T o u t and higher for Experiments 3 and 4. The excess energy obtained with the Experiments 3 and 4 should come from deuterium nuclear fusion reaction. What else explanation exists for this result? Chemical reaction energy is very small and never gives the explanation. We concluded that this should come from fusion. Also it is considered that the "DS-reactor" demonstrated to reach the practical level with high efficiency. It was concluded that the principles of the DS-reactor is the same as that of DS-cell with "DS-cathode", and the "DS-cell" was an excellent system to

52

Outer vessel D 2 /H 2 gas

Pd vessel

The present situation of DS-reactor as the practical reactor of Cold Fusion Generation of nuclear energy inside Pd-vessel

/Nano Pd\ V D2 gas /

(outer vessel)

/Pdblack\ \ D2 gas / Temperature given to outside (D2/H2 gas) (7 0u t> 100°C) of Pd-reactor vessel

® I Pd black\ /Nilo sampleN D 2 gas

^ H2 gas /

- Actual basic line for (sample + D 3 gas) T=

T„+T*„,

/

Tin Never nuclear reaction

Figure 7.

Illustration of "Conclusion".

demonstrate exactly the existence of cold fusion, but gives a bad "efficiency" as a reactor, because in DS-cell, electrolyte is used essentially, then the most of the input energy is consumed inside the electrolyte itself, and then consequently, the "DS-reactor" which is "DS-cell" with no electrolyte will be utilized as a Practical Reactor. 5. Supplement: Measurement System of the Input/Output Power and Characteristics of Reacted Products for the DS-Reactor To keep the constant "giving temperature" (T out = constant), heating current should be changed automatically for the heater with always-const ant resistor. We set a new system to keep the constant "T o u t ", and measured its current transition as shown in Fig. 8, where the input power (W;n) is simply converted by a formula [Win = RI2, R is the constant resistance (50£1) and I is the measured current (A)]. When T out = 140°C, input power was about 1-2 W which is about 1-2% for the DS-cathode, but it is considered that when the radiation loss to the air is protected it will be decreased at the extremely small (%). These results show great characteristics of the DS-reactor as the practical use. Figure 9 shows generation of the much 4 He inside the DS-reactor with D2 gas and Pd black. Above A shows the starting base condition of "QMS" before the

53

Heater controlling system

/^->

Tcout

Heater Sample: Pd black; gas: D2

160-, 140-

0.8 -24

0.7- -22

T ^ n ^

-20

£Jr

7"out

0.6-

10080-

-18

0.5- -16

Current (A)

Temperature (°C)

120-

-14

0.4- -12 0.3-

60-

-10

1

-8 40 H

Current

/

Input power

Win

0.2- - 6

- -4 20-

0-

1

c

50

100

150

200

0.1- 9

•

250

• 0.0- - 0 300

*

Time (min) Figure 8. Characteristics of controlling current (input power) to make the constant "giving temperature".

reacted is injected into the "QMS". The period between B and C shows a part of M4-spectrum of the reacted gas, (the gas volume 5 Torr cm 3 ) which was injected to the special gas tank (volume 2000 cm 3 ) with Getter pump and the high vacuum 10~ 8 Torr, and the gas was kept inside the tank, 3 min, then the gases were injected into "closed QMS" (which was developed and published by us in 1995), And one pair spectrum of M4 (4He, D2) was more exactly shown in the period between C and D. The period from D to E exhibits the spectrums, 15 min, after starting, and remained almost of only He.

54

8x10"

c CD

4x10" 12

Figure 9. Spectral analysis of the inner gases in the "DS-reactor" using sample (Pd black) and D 2 gas. Acknowledgments The authors would like to t h a n k Dr. T. Yokobori, M. J. A. (Emeritus Professor; Tohoku University), Dr. T. Yamazaki, M. J. A. (Emeritus Professor; Tokyo University), Dr. H. Fujita, M. J. A. (Emeritus Professor; Osaka University), Dr. A. Inoue (Vice President, Professor; Tohoku University), and Dr. M. F u t a m a t a (Professor; Kitami Institute of Technology) for their kind cooperation.

References 1. Y. Arata and Y. C. Zhang: Proc. Japan Acad., 70B, 106 (1994); 71B, 304 (1995); J. High Temp. Soc. Jpn. 20, 148 (1994); (Special Vol.) 23, 1-56 (1997); (Special Vol.) 29, 1-44 (2003); Jpn. J. Appl. Phys. 37, L1274 (1998); 38, L774 (1999); 39, L4198 (2000). 2. Y. Arata and Y. C. Zhang: J. High Temp. Soc. Jpn. (Special Vol.) 29, 1-44 (2003); Y. Arata, II Nuovo Saggiatore (Italy phys. Soc) 20, 66 (2004). 3. Y. Arata, Methode of producing ultrahigh pressure gas, US-Patent, No.5, 647, 970 (1997). 4. 21st. Century Science and Technology, Summer (21st Century Science. Associates, Washington DC, 1995), p. 37.

P R O G R E S S IN EXCESS OF P O W E R E X P E R I M E N T S W I T H ELECTROCHEMICAL LOADING OF D E U T E R I U M IN PALLADIUM

V. V I O L A N T E A N D S. M O R E T T I * Associazione

EURATOM-ENEA

sulla Fusione, Centro Ricerche Frascati, Rome, Italy E-mail: [email protected]

Frascati,

C.P.

65-00044

M. B E R T O L O T T I , E. C A S T A G N A , A N D C. SIBILIA Universita

di Roma

"La Sapienza"

Dip. di Energetica.

Via A. Scarpa,

14, Rome,

Italy

F. SARTO ENEA,

Centro Ricerche

Casaccia

Rome,

Italy

M. M C K U B R E A N D F . T A N Z E L L A SRI International,

333 Ravenswood

Avenue,

Menlo Park,

CA 94025,

USA

I. D A R D I K , S. L E S I N , A N D T. ZILOV Energetics

LLC,

7 Fieldview

Lane,

California, NJ, USA or Energetic Industrial Park, Israel

Technologies,

Omer

A research activity has been carried out, during the last 3 years, in the field of triggering anomalous heat effects in palladium deuteride. An enhancement of the excess of power reproducibility in deuterated palladium was obtained by using He—Ne Laser irradiation during electrochemical loading. A preliminary correlation between excess of energy and 4 He concentration increasing above the background was found. The continuation of the experimental program confirmed that Laser triggering produce an interesting gain of reproducibility. An upgrade of the experimental set-up has been realized.

1. Introduction The material science research oriented to improve the effect of excess of power production into palladium cathodes loaded electrochemically with deuterium confirmed that the high concentration of deuterium into the lattice (d/Pd > 0.9) is a necessary condition to observe the phenomenon but not enough. Several research groups have been working in order to identify the most appropriate techniques to trigger *ENEA guest. 55

56

such an effect. The study presented in this work is leading with the development of the triggering by means of Laser irradiation during the electrochemical loading of palladium with deuterium in heavy water electrolyte. An isoperibolic calorimetric system has been developed allowing a Laser irradiation during the electrochemical loading. According to the idea that collective electron oscillations have a key role in LENR processes a proper trigger has been introduced to create surface plasmons (polaritons). 1 Laser triggering was selected because of it results to be the most appropriate under electrochemical loading. Plasmons are longitudinal plasma oscillations that do not couple with external radiation. A proper surface corrugation may produce such a coupling between the electronic oscillation and the external radiation. For such a reason, a proper acid etching has been done on the Pd samples used as cathodes into the electrochemical cell. In addition to that one may consider that a p-polarized Laser beam is the appropriate one to create charge separation on the surface of the specimen. High vaccum cap with electric connections < PT100--

Electrodes rotating support

PT100

SS cap and ring

Glass window for laser beam

Teflon cell

Figure 1.

Electrochemical cell for Laser triggering.

2. Experiments The electrochemical cell (Fig. 1), tested for He leakage (2 x 10~ 10 mbar 1/s), equipped with two small glass windows was placed into a thermostatic box (Fig. 2) (±0.15°C) also equipped with a window for the Laser beam (5 or 33 mW, 632 nm). The closed electrochemical cell is equipped with a recombiner. Cell power supply is an AMEL galvanostat, modulated, during the HI-LO current mode by an HP 33120 wave function generator. Output power is measured by means of the calibration performed by means of the average temperature given by the PT100 thermometers

57

mm wi LCR meter

'—-

1—

Wave generator

....

Temperature monitor Multimeter Data acquisition switch unit

ff-

Laser

Box

Galvanostat Figure 2.

Isoperibolic calorimeter.

located into the electrolyte, R/RQ measurement is done by means of a HP-4284 (four wires measurement). A calibration was done by using light water (0.1 M LiOH) and the calibration curve is shown in Fig. 3. Despites the behavior of the system was quite linear a proper fitting curve has been used in order to have R2 = 1. Three experiments have been carried out into the isoperibolic calorimetric system during the first campaign showing excess of power production during Laser irradiation with "p" -polarization. The produced excess of energy was ranging between 3.4 and 30 kJ. Figure 4 shows the input and output power and energy of Laser 4 experiment. The increasing of He concentration measured with a Jeol GCMate mass spectrometer revealed a satisfactory agreement between the expected value and the measured one by assuming a D + D = 4 He + heat reaction occurring into the lattice. 2 Calibration 25-5-2004 y=-0.1649x= + 5.3626X+ 24.337fl° = 1

60-

^^--Jr'

o S_ 30-

^—* ^^^^"^ —*-T (average)

^ "

- — Pdi. (T (average))

2010-

(

1

2

3

4

5

6

Pin ( W )

Figure 3.

Calibration curve for isoperibolic calorimeter.

58

An improvement of the system was carried out both to increase the number of thermometers into the cell and to use high ultra-vacuum technology for the cap and the glass windows of the cell. A particular effort was done in order to take into account the convective heat exchange due to the electrolyte fluid dynamics due to the gas bubble formation during the electrochemical process. Laser 4 experiment was carried out by applying a continuous electrochemical current. After achieving a loading threshold of 0.95, the cathode was continuously irradiated by using a 632 nm, 33 mW red Laser. Calorimetry gave 30.3 kJ of produced energy (19.4 MJ per mol Pd). Figure 4 shows the input and output power and energy evolution after applying the Laser irradiation. Excess of energy and power in Iaser4 experiment

Figure 4.

Excess of energy and excess of power in Laser 4 experiment.

The gas produced at the electrodes (Pd foil cathode and Pt wire anode) acts on the electrolyte producing a fluid dynamic regime that affects the temperature distribution, then the temperature field for the considered cell results to be correctly described by including the convective terms into the heat transfer equation: dT ( dT dT dT\ div(Xgrad(T)) + Q = pcp— + pcp [Vx— + Vy— +Vz—j,

(1)

with convective external boundary conditions (radiative mechanism is neglected because of the low temperature of the system, close to the ambient one). Assumptions • 3D transient. • Isotropic (Kx = Ky = Kz).

59

• Steady-state boundary conditions (thermostatic box) Tarab = cost. (£). • Radiative heat exchange negligible • Convection of the electrolyte mainly produced by the bubbles formation at the cathode, since the cathode has a reduced area and the deuterium flow rate is twice the flow rate of the oxygen at the anode. In order to reduce the computation time, we propose an approximate solution, in closed form, for the field of velocity. First of all, we have to calculate the velocity of the electrolyte at the interface between the hydrogen and the liquid. The situation is described in Fig. 5.

Figure 5.

Gas-liquid interface at the cathode.

Gas velocity Va2 is calculated by means of the current density. Let us assume the cathode to be a Pd foil having height h and width L. The bubbles of hydrogen form a layer that we measured to be S (2-3 mm) in our cell configuration. The laws of Faraday and of the gas give 22.4 x 1000 cm 3 /s, n = 2.

gas flow rate =

(2)

nF The gas flow rate for unit area is: „ K=

J x 22.4 x 1000 _ , „ = 2.

(3)

By integrating on the whole surface -

JTr-[21n(r/r)-l] 46ln(a/R) '

r

'(15)

The integration constant is calculated by imposing the condition of zero flow rate in radial direction

2nh /

vr dr = 0 that gives the value of C I R :

(16)

Ja

IK

ClR

a2-R2+a2HR/a)

^"4T

jj^jf

'

(17)

Step 3: By replacing again vr(r) into the continuity equation we obtain VVz(r,z), the integration constant is calculated by considering now zero flow rate into the axial direction VVz(r,z) = -zK2ln^+Clz, 2?r / VVz{r,z)rdr = 0, Ja \ „ (a2-R2 + 2lnR/a)

2* 2 * 1

n£

IJ

^W

(18) (19)

62

Ifl

J~~l_

sX Temp on

0

3

max: 314.9 q: 314.0 p: 313.0 o; 312.0 n: 311.0 m: 310.0 I: 309.0 k: 308.0 j : 307.0 i: 306.0 h: 305.0 g: 304.0 f; 303.0 e: 302.0 d: 301.0 c: 300.0 b: 299.0 a: 298.0 min: 297,7

6

Y

Figure 7.

Temperature field into the cell (isotherms).

The two components of the liquid velocity are VVz and Vr Cm *(') = VVz{r,z)

Kr[2\n(r/R)-1] ASHa/R)

= -zK2ln(r/R)

+ Clz,

'

IK 45

Cl R

1 2

d

— J\oZ

a2 - R2 + a2 hx(R/a) [\n(R/a)]' (a2 -R2 + 2 In R/a) — a? -R

(21) and describe the velocity field into the electrolyte (see Fig. 6). A three-dimensional (3D) transient finite element analysis gives the field of temperatures into the cell, Fig. 7 shows the temperature distribution into the electrochemical cell. Figure 8 shows the comparison between the experimental results and the calculations, the comparison reveals a satisfactory agreement when the fluid dynamic

Model

p

*- Model without fluid-dynamics a - Experiment it- Model no fluid-dynamics

P(W) Figure 8.

Comparison between model results and experimental data.

63

of the electrolyte is included into the system description, in particular for power values larger t h a n 2 W. A new experimental campaign has been carried out giving one excess of power production over two experiments. T h e excess of power is shown in Fig. 9. T h e effects started after achieving a loading around D / P d = 0.94 and survived, under Laser irradiation for more t h e n 100 h. T h e maximum gain was about 15% of the input. T h e excess was stopped by current inversion t h a t produced a fast de-loading. After de-loading the difference between the input and the o u t p u t power disappeared. T h e effect is clearly shown in Fig. 9. T h e total energy gain was 49 kJ.

149 kJ excess of

Current

0.9 0.8

"W.WW

0.7

R/Ro


=5

100

0) Q.

E 2 cf data ¥W 40803 # 1 Figure 4.

2.8. Mass

4 Time (1000 s)

Changes of voltage, cell temperature, and current.

Analysis

The generated gas was continuously analyzed a quadrapole mass analysis. A small amount of gas was introduced into a differential evacuation system and then brought to the mass analysis measurement system. We used mass analysis of Ulvac Rega-201 that is a mass filter type of Quadrapole mass analyzer. The analyzer can measure mass number from 2 to 400. 3. R e s u l t s a n d Discussion Figure 4 shows the changes of input voltage, cell temperature, and current for a typical experiment. Input voltage was usually increased stepwise from 0 V to more than 100 V and then decreased to 0 V. The input current usually rose to a maximum

71

Parameter change 100

>

6

— Cell temp.

80

0)

2

60

C

ro O

llf ro a. £

/

-

V

4

Current (A)

i

•-

3

40

2

^

S 20

|2

/•

0 1! 0

/

i

i ^

15 0

1

//' i

I""""""1 A

• 1

i

190

210

'u 250

2. 0

!ime(s)

Figure 5.

Time expanded graph of Fig. 4.

value of 4.3 A during conventional electrolysis with 1 cm 2 area of W electrode, but it usually decreased once plasma started, and stayed around 1.6 A when voltage ranged from 120 to 220 V. The time-expanded graph of Fig. 4 is shown in Fig. 5. It indicates input voltage, current, and temperature changes for the first 250 s in Fig. 4. Here, input voltage is increased at 182 s and reached to 40 V at 220 s, and at the same time, current increased to 1.8 A. Meanwhile, electrolyte temperature raise is within Idegree, it can be say almost constant.

100

f

80

— Terr

t»

>

5

I

J\ I

-- Cur 60

-Volt

1

1 J- \

20

1

n

c

23

| ddaia\\V»l24«l |

Figure 6.

\

A0

\

V^

1

40

!

4

3

g 3

2

>

1

. * ,

60

i

80

0 1 )0

Time (s)

Changes of voltage, cell temperature and current.

72

Changes of input and output 1E + 05

t

/

1E + 0 4 k

5

B"3 o 1

•#• Input

/

F 1E + 03

-©-Outpu t

/ /

| / 1E + 02

i /

1E + 01 y

L

J

1

# ;*A

20

1

L_L_

1

40

60

1

L

80

1 100

Time (s)

rcfdata\W50l24#l I

Figure 7.

Changes in input and output heat.

However, the changes of temperature during the explosive reaction were different from the usual experiment. The input voltage and current were 15 V and 1.5 A at 40 s, respectively; that equals 22.5 W, as shown in Fig. 8. The input power was supplied for 10 s; total input was roughly 300 J. The electrolyte temperature rose steeply from 40 to 60 s, within 20 s. After that, the electrolyte cell was shattered by the sharp increase of inner pressure. The heat out was estimated 800 times higher than the input power, based on the remaining output data. , i s o T e + 5 6

F e+

- • 136Xe +50

-> -• -•

138

128_6

C r+ n

7

M e V

4

Me

y

48

B a + T i + 1 1 7 . 4 MeV Ce + 4 4 Ca + 107.2 MeV 154 S m + 3 2 S + 7 9 . 2 MeV 142

^158Gd+28gi+727MeV

However, it is still difficult t o explain the reaction by this mechanism, because of the absence of heavier pair elements.

References 1. Tadahiko Mizuno, Tadayoshi Ohmori, Tadashi Akimoto, and Akito Takahashi, Production of heat during plasma electrolysis in liquid, Jpn. J. Appl. Phys. 39, 6055-6061 (2000). 2. Tadahiko Mizuno, Tadashi Akimoto, Kazuhisa Azumi, Tadayoshi Ohmori, Yoshiaki Aoki, and Akito Takahashi, Hydrogen evolution by plasma electrolysis in aqueous solution, Jpn. J. Appl. Phys. 44(1 A), 396-401 (2005).

"EXCESS HEAT" I N D U C E D B Y D E U T E R I U M FLUX IN PALLADIUM FILM

BIN LIU, X I N G Z. LI, A N D Q I N G M. W E I Department

of Physics, Tsinghua University, Beijing E-mail: [email protected]

100084,

China

N. M U E L L E R , P. S C H O C H , A N D H. O E H R E Inficon

Limited,

Alte Landstrasse

Principality

of

6, LI-9496

Balzers

Liechtenstein

An early work at NASA, USA has repeated at INFICON Balzers, Liechtenstein in 2005. It is a confirmation of the correlation between excess heat and deuterium flux permeating through the Pd film. The maximum excess power density is of the order of 100 W / c m 3 ( P d ) .

1. Introduction Early in 1989, G. C. Fralick et al., of NASA, USA conducted an important experiment to search for the neutron radiation using gas-loading method in a D/Pd system instead of electrolysis.1 They could not find any evidences for the neutron radiation in a D/Pd system; however, they discovered unexpectedly the "excess heat" in a D/Pd system. Thanks to J. P. Biberian, we became aware of this NASA work after ICCF-11. This NASA experiment was very similar to our gas-loading experiments, which have been conducted at Tsinghua University since 1989. 2 ~ 4 The excess heat appeared in both our experiments and in NASA experiments whenever deuterium gas was pumped out from the Pd samples. In our early work,2 we used palladium wire only and heated Pd wire using the electrical current through it. G. C. Fralick et al. utilized the Pd-alloy tube in a hydrogen purifier, and heated this tube using an external electrical heater from outside of tube. Nevertheless, in W. Wu and X. Z. Li's work,3 we utilized Pd tube also, but we heated the Pd tube using electrical current through Pd tube. This is different from Fralick's heating from external heater. On the other hand, X. Z. Li and J. Tian 4 were using an external heater, but the pumping was done only at one side of the Pd tube. However, G. C. Fralick et al. pumped deuterium gas from both sides of the Pd-alloy tube. We now use a Pd disk heated by an external heater, and pump down from both sides of the Pd film (Fig. 1). Although the configuration varied in various experiments, the results are all similar, i.e., the "excess heat" appears while a deuterium flux leaving palladium is created. 75

76

Swagelok connection Thermocouple Heating coil

Figure 1. A thin palladium film is sealed between two tubes using a Swaglok connection structure. There are two small holes on the nut. Thermocouples are inserted into holes in order to measure the temperature of the edge of the Pd film. The heating coil winding is wrapped around the nut to hea.t the Pd film.

2. N A S A ' s Early Gas-loading Experiment In a hydrogen purifier (HP-25, commercial available through Johnson & Matthey Inc., Fig. 2), 13.8 atm. deuterium gas was fed into the palladium tube from both the inner side and outer side. It was heated electrically to 383°C. When the deuterium gas was pumped out using the mechanical pump, the temperature of the palladium tube increased suddenly from 383°C to 400°C in 15 s. It was not caused by the reduction of heat conductivity, because there was no such temperature variation when hydrogen gas was fed instead of deuterium gas. It was further confirmed by switching off the electrical power before starting the pump. In this case, the temperature dropped from 374°C to 370°C and then slowly increased back up to 375°C, again indicating the heating as the deuterium was removed from the palladium. As before, no neutrons were registered by either detector during the time the heating occurred.

Figure 2. Hydrogen purifier is utilized as a palladium tube-deuterium system with heating element wrapped in the insulator. The helical stainless tube on the top is for cooling the purified gas.

77

With the assistance of INFICON R&D Laboratory, this NASA experiment was repeated and the gas sample was analyzed using high-resolution quadruple mass spectrometer. This paper would report the result of excess heat first. The result of quadruple mass spectrometer analysis would be reported in another paper. 5 3. Tsinghua INFICON Collaboration Early in 1989, the hydrogen purifier was an existing equipment for NASA scientists to study the D/Pd system; however, it was not easily accessible for us in 2005. With the assistance from IERA, 6 we had experience in running Swagelok connection like that in Fig. 1. The advantage of this configuration was that it was easy to utilize the high-resolution quadruple mass spectrometer in the INFICON R&D Laboratory in order to identify the nuclear products from the D/Pd system. A Pd film with high purity (99.98%) was cut to be fit into the Swagelok connection. It was about 20 mm in diameter and 0.1 mm in thickness. The Pd film might be heated to 330°C using the electrical heater wrapped around the nut. The temperature of the Pd film might be monitored by the thermocouples inserted into the holes on the nut. The system was pumped to 10~ 6 mbar. Then the deuterium gas was filled into the system to 999 mbar. The electrical heater was turned on to heat the system from 25.3°C to 330.2°C in 1.5 h using '--113 W heating power while the room temperature is about 23.6-25.0°C. During the heating the deuterium pressure dropped first because of the strong absorption of the Pd film. The pressure was down to 996 mbar first; then, it increased slowly due to the heating. When we started pumping, the pressure was 1004 mbar. The Pd temperature started increasing when we started pumping as that seen in Fig. 3. When pressure was down to 0.1 mbar, the decreasing rate of pressure slowed down. An additional turbo-molecular pump was turned on at that time. The pressure was further down to 10~ 4 mbar. A very clear temperature rising was observed in this period. The temperature reached the highest point (339.8°C) after 70 min; then, it started decreasing even if the pumping continued to pump the pressure down to 10~ 5 mbar. This behavior was very important in order to exclude the effect of the heat conductivity. Usually, we might worry about that the heat conductivity might drop while the gas pressure dropped. Indeed, this last period just showed that the effect of heat conductivity in this temperature rising was not important. The electrical heating power was provided by a VARIAC power supply. It showed a stable voltage about 221.2 V(AC). We might worry about the room temperature fluctuation. It was monitored by a thermocouple and a mercury thermometer. The lowest was 23.1°C, and the highest was 25.0°C. 4. Discussion The absorption of deuterium gas into palladium is an exothermic process. Hence, the degassing of deuterium from the palladium is supposed to be an endothermic process. We were supposed to observe the temperature drop when we started pumping. This was true, when the data acquisition system was able to catch that

78

short temperature drop just after the starting point of pumping. It was caused by both the endothermic degassing and the adiabatic expansion. However, this short drop in temperature was always followed by a temperature rising which was corresponding to the correlation between heat and deuterium flux. This phenomenon was discovered in the study of gas-loading in palladium wire, 2 and was named as "pumping effect". The careful study using high precision calorimetry confirmed this phenomenon, and called it as correlation between heat flow and abnormal deuterium flux.3,4 The early NASA gas-loading experiment provided a strong evidence to this phenomenon unexpectedly.1 The collaboration with INFICON R&D laboratory has made us even more confident about this phenomenon. Deuterium flux and excess heat 340-

10,000

Start pump ingj' i

^

** / ,

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/

1000 100 10

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20:09 20:38 21:07 21:36 22:04 22:33 23:02 23:31 24:00 24:28 24:57

Time

Figure 3. Solid line shows the temperature at the edge of the Pd film. Dash-dotted line shows the pressure around the Pd film. The temperature started increasing when pumping was started. However, temperature dropped later even if the pumping was continuing.

We may estimate the excess power in this pumping period. The resistance of the heater was 433 fi at 330°C, it provides an effective heating power of 113 W at 221.2 V. This heating power was able to maintain a temperature difference of (330.2-24.0) = 306.2°C. Hence, the temperature difference of (339.8-330.2) = 9.6°C might imply an "excess power" of 3.5 W. The volume of the Pd film was about 0.031 cm 3 ; hence, the power density for the palladium was about 114 W/cm 3 . It is about the power density in a modern nuclear fission reactor. Acknowledgments This work is supported by the Natural Science Foundation of China (No. 10475045), Ministry of Science and Technology (Division of Fundamental Research), and Tsinghua University (985-11, Basic Research Funds). References 1. G. C. Fralick et al., Technical Memorandum 102430 (1989). 2. X. Z. Li et at, The Proceedings of ICCF9, Beijing, China, May 19-24, 2002, Edited by Xing Z. Li, Tsinghua University Press (2003), p. 197.

79

3. W. Wu and X. Z. Li, Proceedings of ICGF9, Beijing, China, Mayl9-24, 2002, Edited by Xing Z. Li, Tsinghua University Press (2003), p. 412. 4. X. Z. Li et al, J. Phys. D: Appl. Phys. 38, 3095 (2003). 5. Q. M. Wei, Xing Z. Li, Bin Liu et al., High resolution mass spectrum for deuterium (hydrogen) gas permeating palladium film, The Proceedings of ICCF12, Nov. 27-Dec. 2, 2005,Yokohama, Japan, Edited by A. Takahashi, Y. Iwamura, and K. Ota, World Scientific (2006). 6. X. Z. Li, G. L. Schmidt, and J. Tian, The Proceedings of the 5th Asti Workshop on Anomalies in Hydrogen/Deuterium Loaded Metals, March 19-21, 2004, Asti, Italy.

A B N O R M A L EXCESS HEAT OBSERVED D U R I N G M I Z U N O - T Y P E EXPERIMENTS

JEAN-FRANgOIS FAUVARQUE, P I E R R E PAUL CLAUZON AND G E R A R D JEAN-MICHEL LALLEVE Laboratoire

d'Electrochimie Industrielle, Conservatoire National rue Saint Martin, F-75141 Paris Cedex 03, E-mail: [email protected]

des Arts et Metiers, France

292,

A simple calorimeter has been designed that works at constant temperature; that of boiling water. Heat losses can be estimated accurately with an ohmic heater. As expected, losses are independent of the electric power input to the heater and the amount of evaporated water is linearly dependant on the power input. The device has been used to determine the heating power of a plasma electrolysis (the Ohmori— Mizuno experiment). We confirm that in this experiment, the heat output from electrolysis is greater than the electrical power input. The excess energy increases as the electrolysis voltage is increased from 200 up to 350 V (400 W input). The excess energy may be as high as 120 W.

1. Introduction Our experiment is an electrolysis experiment made in plasma mode with a tungsten cathode, a platinized titanium wire as an anode, and as electrolyte a water solution of potassium carbonate (K2CO3 at 0.2 M). In the same type of experiments, Mizuno 1 ' 2 reported both excess heat and excess hydrogen production. The explanations found in the bibliography for this phenomenon are, for example, transmutations in the cathode material. 3 The abnormal observations are concerned with the appearance of osmium, iridium platinum, and gold, without quantitative measurements. 3 We thought it would be quite interesting to confirm these results with the help of a simplified experimental setup. 2. Experimental We decided to do our experiments at a constant temperature, the boiling point of water, and to measure the heat emissions only by weighing the mass of water in the experimental device. A water storage container inside the device allows us to maintain the electrolyte at a constant water level, and thus keep the K2CO3 concentration constant. This container, being graduated, also gives us a way to confirm the mass of water boiled off. An interesting repercussion of this operating mode concerns the thermal losses. Once the boiling temperature is reached and overall thermal stability is achieved, 80

81

the thermal losses, which depend only on the temperature, remain constant, and this is true whatever thermal emissions are observed. This allowed us to hold the experiment in a simple beaker of an appropriate size and then to avoid the of an opaque Dewar vessel. This allows us to visually observe the cathode condition. Finally, the use of an ohmic heater allowed us to bring the device at the suitable boiling temperature and to maintain this temperature at this level much more quickly than by electrolysis alone. We also verified that other sources of inaccuracy were insignificant. For example, in the range of power used, the recondensation level inside the device was low, and few unboiled droplets of water sprayed outside the beaker. The excess heat that we were trying to measure is quite large (30-100%). So, it is not necessary to obtain very precise measurements. 3. Experimental Device Description Figure f shows the details of the experimental setup: • A SARTORIUS balance, the heart of the device, measuring up to 6 kg at an accuracy of 0.1 g. • Beaker containing between 1 and 1.51 of electrolyte. • Tripod (not shown in this figure) is placed on the balance to hold the electrodes and a container of pure water. • Continuous current electricity supply (500 V, 4 A). • Wattmeter to measure the input energy (Unigor 390 LEM).

Glass tube Distilled water reserve

Anode4

Ohmic heater Electrolyte reserve ((Sartorius)},^balance

1

i

ooo.o g

Figure 1. Experimental setup. Electrolyte reserve is 2 1. The tripod used to hold components in position is not shown.

82

Figure 2.

Photograph of the experimental apparatus.

The input energy was also frequently measured by use of the inlet voltage and the mean current intensity as given by a recorder. These results were compared the wattmeter data. ® A tungsten cathode of 2.4 mm diameter made with 2% of thorium (this type of electrode is often used for commercial scale welding). This cathode rod is shielded with a Pyrex tube. About 15 mm of the rod extends out from the tube, where it is exposed to electrolysis. In some experiments, ceramic tubes were used instead of Pyrex. ® An anode made up of a wire in platinized titanium in a cone or cylinder shape around the cathode to regulate the water current. This is made quite large, to cope with the boiling, and to stop unboiled droplets of electrolyte from leaving the beaker. The anode and cathode are 4 cm apart. ® An ohmic heater rated to about 400 W (enough to evaporate 34 g of water in 300 s). ® A distillated water container equipped with a tap, which allows us to maintain a stable water level inside the beaker during the experiment. ® Various measuring instruments for the electrical components. A typical run lasts 10-20 min, divided into 5 min measurement periods. The evaporated water quantity may reach 50-100 g, which corresponds to energy ranging from 113,000 to 226,000 J. In some cases, we used a Geiger-Muller device to check for possible nuclear radiation. The results of these nuclear observations were always negative (Fig. 2).

83

4. Results and Discussion 4.1.

Calibration

Using an ohmic heater, which can remain inside the beaker permanently, we have verified the response of our device to heat emission. It was necessary to verify that the thermal losses were constant beyond a certain input power level, and then that every increase in power would give a loss of water corresponding exactly to the energy supplied in the device during the measurement period. The electrolyte level is maintained constant, due to the supply of water (at 20°C) from the reserve. The energy used for the boiling of 1 g of water is then: 2260 J (latent heat at 100°C) + (100°C - 20°C) x 1 x 4.18 (heat needed to bring l g of water from 20 to 100°C) = 2594 J. Figure 3 shows the results. Note that from about 300 W inlet power, the experimental curve and the theoretical straight line are rigorously parallel, and the thermal loss is 75 W. Three important features can be deduced when we maintain the power of the ohmic heater at about 400 W. We were able to verify the validity of our measurement of the latent heat of water evaporation. The power increase due to the experiment is directly measured by the water loss during a given time unit. Losses due to the recondensation inside the experimental device, as well as those caused by unboiled droplets driven out of the beaker, seem to be negligible. 4.2.

Results

We made a parametrical study on the influence of the voltage applied during glow discharge electrolysis. The temperature was brought to the boiling point (100°C)

Vaporized water with re-feeding 700 600

«

400"

0- 300

30

40

m (g/300s) Figure 3.

Device calibration using ohmic heating only.

84

with the auxiliary resistance heater. Then electrolysis was begun at 200 V. This high voltage is needed to produce a suitable plasma around the cathode. Plasma generation is greatly enhanced by the high-electrolyte temperature. The Joule heating effect during electrolysis immediately gives rise to an envelope of steam around the cathode, and a plasma, that is supposed to be hydrogen plasma according to Mizuno. Table 1 gives the value of the COP, which is the ratio of the energy of vaporization divided by the electrical energy supplied to the device (which of course includes energy consumed by the ohmic heater). It is very important to confirm that the device is thermally stable. The selected definitive values for the inlet energies are the values of the wattmeter, considered to be more reliable than those based on voltage and mean registered current. Table 1.

4.3.

Five-minute test results

Voltage (V)

COP (energy out/energy in)

Number of tests

200 250 300 350

1.0 1.05-1.12 1.12-1.15 1.31-1.41

3 8 8 4

Remarks

(1) The calculation of the COP is straightforward. Let us take the 200-volt data. The mass of evaporated water is 63 g, with for 34 g due to auxiliary resistance heater. The mean current was 1.25 A, and the duration of the test is 300 s (5min). Energy out: 63 g - 34 g (auxiliary resistance) x 2594 J = 75,226 J. Energy in: 200 V x 1.25 A x 300 s = 75,000 J. The COP is then: 1.0. (2) The COP values bands are not correlated with the inaccuracy of the measurements. The results presented here were collected over several hours of operation of the cathode. The cathode is corroded at the very high temperatures of the experiment, so between experimental runs we push more of the cathode through the Pyrex shield, keeping the length of exposed cathode at about 15 mm. That explains the variation bands. (3) Reproducibility is within a range of about 5%. 4.4.

Discussion

The very simple device used allowed us to highlight with reproducibility an abnormal excess heat, which increases with voltage. We believe that we have confirmed abnormal excess energy for voltages higher than 200 V with our present device. The data presented here for 350 V correspond to input power exceeding 400 W. The abnormal excess heat exceeds 120 W without

85

taking into account the gas formation or luminous radiation. This power is therefore definitely significant. We did not find any classical explanation for this thermal effect, and we are examining the possibility of less classical explanations. 5. Conclusion The initial purpose of these experiments was to investigate the potential of a simple experimental device to confirm the results obtained by Mizuno. 1 ' 2 We think that this first step has been accomplished and that we can say that ratios between output and input energy (COP) of 1.3 and 1.4 have been reached with satisfactory reproducibility. In a second step, we will try to explain this phenomenon in order to increase the COP. In any case, the device presented in this paper is a very simple device, which can be used to rapidly verify hypotheses without sophisticated means. For example, we have verified that this phenomenon does not seem related with the heavy water, which is found at one part in 7000 in natural water. We increased the concentration of heavy water by a factor of 100 in our electrolyte, i.e. to 1 part in 70. We did not see any perceptible change in our results. Acknowledgments The authors want to express our deep appreciation to M. M. D. Noel, J-L. Naudin, and O. Horner of "EDF Les Renardieres" for fruitful discussions. References 1. D.Y. Chung, Y. Aoki, F. Senftle, and T. Mizuno, ICCF11 Conf. (Marseille, 2004). 2. T. Mizuno, T. Akimoto, and T. Ohmori, Fourth Meeting of Japan CF Research Society (Iwate University, Japan, 2003). 3. D. Cirillo, A. Dattilo, and V. Iorio, ICCF11 Conf. (Marseille, 2004).

SEEBECK E N V E L O P E CALORIMETRY W I T H A P d | D 2 0 + H 2 S 0 4 ELECTROLYTIC CELL

W U - S H O U ZHANG, 1 " J O H N D A S H , A N D Q I O N G S H U W A N G Low Energy

Nuclear

Laboratory, Portland State OR 97207-0751, USA E-mail: dashj@pdx. edu

University,

Portland,

Anomalous excess heat in P d | D 2 0 + H2SO4 electrolytic cells was confirmed using an accurate method of heat measurement, Seebeck Envelope Calorimetry. A cell was placed in the calorimeter, which measures the output heat flux directly and avoids many of the problems other methods have. The maximum excess power thus far was 1.3 W (or 11 W / c m 3 ) with input power of 13 W at a current density of 0.4 A / c m 2 . Calibrations were carried out before and after electrolysis experiments using a P t | H 2 0 + H2SO4 electrolytic cell, a dummy cell with inner resistor, or a pure resistor. Different calibrations gave consistent device constants within experimental error. Pd cathodes were analyzed by scanning electron microscopy and energy dispersive spectrometry. Unexpected elements were observed on the sample surface after electrolysis.

1. Introduction After the successful public demonstrations of excess heat in Pd|D20 + H2SO4 electrolytic cells at Boston (ICCF10) in 2003,1'2 we confirmed this anomalous effect using a more accurate calorimeter: a Seebeck Envelope Calorimeter (SEC). The SEC is a cube; the electrolysis cell is placed inside it. The SEC converts the heat flux through the six walls of the cube into a voltage signal using many thermocouples distributed uniformly in the walls. Many problems of isoperibolic calorimetry and mass flow calorimetry can be avoided by this method. 3,4 In this report we present the calorimetric results for the Pd|D20 + H2SO4 electrolytic cell, results with Ti added to the D 2 0 + H2SO4 electrolyte, and the results of analysis of the Pd cathodes. 2. Experimental Setup Closed cells are similar to that used before1'2 except that the height is less in order to fit into the SEC as shown in Fig. 1(a) and described below. The electrolytic cell is a Pyrex cylinder (capacity is about 280 ml, 4>-m = 50.7 mm and !>i.„nm 489.5

482.8

476.1

X

3

650

660

670

im

680

Figure 9. Spectra of two measured lines of hydrogen radiation of the sonoluminescence area. T h e possibility of the realization of one of the most optimal fusion reactions: p + B —» 3He for these liquids was investigated. T h e process of He 4 creation was investigated by the analysis of the optical spectrum of luminescence of the stationary plasma jet and identification of He spectral lines in real time. One of the main problems of identifying such reactions is connected with the search for an optimal method of controlled B 1 1 isotope insertion in the cavitation zone. Experiments have shown t h a t uncontrolled insertion of ions of B 1 1 isotope as an admixture leads to suppression of the sonoluminescence. T h e possibility of the realization of reactions of the carbon-nitrogen cycle in moving turbulent machine oil was also investigated. These processes were studied using various nuclear and spectral methods, including correlation analysis of the radiations from the luminescence region. In several cases the generation of directed intense hard X-ray (or gamma-ray) beams was detected outside the working chamber with cavitating machine oil or distillated water. This hard irradiation was detected using X-ray photographic plates t h a t were isolated in black paper and fixed on the external surface of the plexiglas working chamber. Initial calorimetric tests have shown t h a t the final (output) thermal energy of hot circulating machine oil in some cases exceeds the input electrical energy used for liquid pumping. These results, including studies of nuclear t r a n s m u t a t i o n and energy release, will be reported in the near future following additional research. References 1. V. I. Vysotskii, On possibility of non-barrier dd-fusion in volume of boiling D2O. Proceedings ICCF4, 1994, 4, pp. 6-1-6-3. 2. V. I. Vysotskii, Conditions and mechanism of non-barrier double-particle fusion in potential pits. Proceedings ICCF4, 1994, 4, pp. 20-2-20.5. 3. V. I. Vysotskii and R. N. Kuzmin, Nonequilibrium fermi - condensate of deuterium atoms in microcavity of crystals and the problem of nonbarrier cold nuclear fusion realization, Soviet Phys. - J.T.P. 64(7), 56 (1994).

107 4. V. I. Vysotskii and A. A. Kornilova, Nuclear Fusion and Transmutation Biological Systems. Moscow, "MIR" Publishing House, 2003. 5. D. J. Plannigan and K. S. Suslick, Nature 434, 52 (2005). 6. B. P. Barber et al, Phys. Report 281, 65 (1997). 7. W. B. NcNamara et al, Nature 401, 772 (1999). 8. K.Yasui, Phys. Rev. Lett. 83, 4297 (1999). 9. O.Baghdassarian et al, Phys. Rev. Lett. 86, 4934 (2001).

of Isotopes in

D E S C R I P T I O N OF A SENSITIVE SEEBECK CALORIMETER U S E D FOR COLD F U S I O N STUDIES

EDMUND STORMS Lattice Energy, LLC, Santa Fe, NM, USA E-mail: storms2@ix. netcom.com A sensitive and stable Seebeck calorimeter is described and used to determine the heat of formation of PdD. This determination can be used to show that such calorimeters are sufficiently accurate to measure the LENR effect and give support to the claims.

1. Introduction Heat production is an essential feature of the cold fusion effect and its measurement has been a frequent object of criticism.1 Since 1989 when Profs. Fleischmann and Pons (F-P) 2 first revealed their observations, calorimetry has evolved from the simple isoperibolic design and become increasingly accurate 3 with use of the Seebeck type. 4 " 7 The Seebeck (Kelvin) calorimeter consists of thermal-electric converters that completely surround the source of heat. Temperature at the outside of these converters is held constant while temperature at the inside is allowed to increase. The average temperature difference generates a voltage that is used, after calibration, to determine the rate at which heat passes through the thermal barrier created by the converters. Because the design is very simple, operation is easy to understand and potential errors are easy to determine. When used in a study of cold fusion, a gas-tight glass cell containing an electrolyte and electrodes is placed in the enclosure. Because the measured voltage represents an average of heat loss through all parts of the barrier, the device is only slightly sensitive to where the cell is placed within the enclosure. A fan is used to distribute heat more evenly and to reduce the cell temperature by removing heat from it more rapidly. The calorimeter is completely insensitive to where heat is being generated within the cell. A calorimeter suitable for measuring the cold fusion effect must be sufficiently sensitive to detect a few tens of milliwatts superimposed on tens of watts. In addition, it must remain stable over long periods of time. The method of calibration must define the same characteristics as when heat is produced by an unknown source. Power production can be calibrated by generating heat using a resistor contained in the device. A dead cell or conditions expected to produce no anomalous energy can also be used. If the calorimeter is sufficiently sensitive, the total amount of energy given off by a known chemical reaction can also be measured. In this 108

109

work, power is calibrated using a resistor in the cell or by using a Pt cathode and a quadratic equation, watt = A + B x V + C x V 2 , shows the relationship between generated voltage (V) and applied watts (W). In addition, the calorimeter is used to measure the total amount of energy absorbed when a Pd cathode is loaded with D. Because this quantity is well known, 8,9 the method gives further demonstration that the calorimeter is indeed accurate and able to detect small amounts of energy. Defining the accuracy of a calorimeter using a few numbers is not practical because several different and independent potential errors exist. Because of bubble action at high current, the amount of power being applied to a F^P cell is noisy. In addition, use of a fan adds additional noise, especially at low applied current as is the case during this study. This causes random fluctuations in measured power, which are as much as ±10 mW during this study. If this fluctuation is too great, it can mask small changes in anomalous power, but it does not introduce an error that might be interpreted as anomalous power. On the other hand, the calibration constant or the sensitivity of the calorimeter can change with time. These changes can be produced by changes in reference temperature, in room temperature, in the amount of recombination taking place in the cell, or in physical parameters when new samples are placed in the cell. This potential drift is the main source of incorrect results. These potential errors are explored in this work. 2. Description The device described here is made by gluing together commercially available thermoelectric converters, as shown in Fig. 1, using waterproof epoxy glue. The panels are connected electrically in series. Once assembled, the outer surface is covered with an electrically insulating, waterproof epoxy paint. The electrical resistance of this coating must be tested and found to be high (>1 Mohm) before final assembly. If the resistance is too low, unwanted voltages will be generated by chemical reaction between the cooling water and the metal plates. These assemblies

Figure 1. Glued panels assembled into two haves of a calorimeter. The length is 13.9 cm, the width is 6.9 cm and the total depth when assembled is 14.8 cm.

110

Figure 2. Assembled calorimeter with \vat• % - * - ~ „- *r - - , S&^<J,fiuio< 2.50 -0 50.00 -1 tv ) 5 10 15 20 25 30 35 40 45 50 55 60 65 70 75 80 85 90 •«*• Penstock [bar] — Draftjubel [bar]^Draft„tube2 [bar]™ Speed_U4[%] «~S.M. opening_U4[%] •— Headcover press, [bar] — Flap gate pressure [bar] — Air press, vessel [bar] Air press, a. valve [bar] Deflection [mm]

_"

Figure 4. gates.

_

,_ _

200.0 190.0 180.0 170.0 160.0 150.0 140.0 130.0 120.0 110.0 100.0 90.0 80.0 70.0 60.0 50.0 40.0 30.0 20.0 10.0 0.0

Several examples of TCB jet plasma generation by opening and closing of the wicket

5. Conclusion A helical cavity, which is formed in hydropower plants during load rejection, can collapse, and violent TCB jet plasma can be implanted. It appears possible to

170

simulate these phenomena (load rejection). Its energy is achievable and controllable. T h e level of collapse energy and frequency is controllable by the use of air injection. It is possible to generate T C B jet plasma when the wicket gates open and close several times during load rejection.

Acknowledgment T h e author would like to t h a n k J. Rothwell from LENR-CANR.org for his editorial and technical comments.

References 1. R. Stringham, Cavitation and fusion, in: Tenth International Conference on Cold Fusion (2003). 2. R. Stringham, Pinched cavitation jets and fusion events, in: The Ninth International Conference on Cold Fusion, Condensed Matter Nuclear Science (Tsinghua University Press, Beijing, China, 2002). 3. X. Wang, M. Nishi, and H. Tsukamoto, A simple model for predicting the draft tube surge, in: XVII IAHR Symposium, Section on Hydraulic Machinery and Cavitation, Beijing (1994). 4. M. Tunc and F. Delale, Energy dissipation due to fission of cavitating bubbles, in: Fifth International Symposium on Cavitation (Osaka, Japan, 1-4 November 2003).

N E W RESULTS A N D A N ONGOING EXCESS HEAT CONTROVERSY

L. KOWALSKI Montclair State University, Montcalir, NJ, USA E-mail: kowalskil@mail. montclair. edu G. LUCE AND S. LITTLE EartchTech Inc., Austin, TX, USA E-mail: [email protected] E-mail: UttleQearthtech. org R. SLAUGHTER Advanced Energy Industries, Fort Collins, CL, USA E-mail: rslaughterQcompuserve. com

Mizuno-type cells (glow discharge plasma electrolysis) were used to measure excess heat generated at several potentials between 250 and 650 V. No significant amounts of excess heat were detected. That conclusion contradicts findings of several researchers.

1. I n t r o d u c t i o n This report describes results of two separate experiments, one conducted in the EarthTech laboratory (Austin, T X , USA) and another in the laboratory of Richard Slaughter (Boulder, CL, USA). T h e purpose was to either confirm or refute reality of excess heat in a plasma electrolysis cell. Our experimental setup was similar to t h a t of Fauvarque et al.1 It is a jar with an electrolyte (K2CO3, 0.2 M) containing two electrodes: a cylindrical anode (platinized niobium) and a tungsten cathode (welding rod). A constant difference of potential, for example, 400 V, is applied to electrodes and a glowing layer of gas is formed around the cathode. Three parameters are measured during each test: the electric energy delivered to the cell, E, the amount of heat lost through water evaporation, Q i , and the amount of water lost through conduction and radiation Q2. T h e difference between Q i + Q2 and E, if any, is called excess heat. As in Ref. 1, our experimental results are reported in terms of the coefficients of performance ( C O P ) . T h a t coefficient is simply the ratio (Qi+Q2)/£171

172

2. Experimental Results According to Ref. 1, the COP, at 350V, is approximately 1.35. Our results, 2 ' 3 shown in Table 1, conflict with that conclusion. Table 1.

Coefficients of performance at several voltages

Volts

250

250

300

300

300

355

350

350

400

650

COP

1.00

0.99

0.97

1.00

1.00

1.02

1.03

0.98

1.05

1.05

The first nine results are based on experiments performed in Texas 2 ' 3 , the last result is based on experiments performed in Colorado. 4 The Colorado setup was similar, in principle, to that in Texas except for the power supply (see Appendix 1). An important observation concerning both experiments can be seen in Appendix 2. The Colorado experiment was simply a 21 beaker, mounted on a balance, with two electrodes. Another difference between our two experiments was that the diameter of the anode in Texas was 6 cm while in Colorado it was 3 cm. The range of potential differences in Colorado was from 500 to 700 V. The mean value of COP in that region turned out to be 0.90±0.2. The last value 1.02, shown in Table 1, resulted from eight separate tests. The standard deviation calculated from these tests turned out to be 0.11. It is interesting that foaming and splashing in Colorado was so insignificant that an experiment could be conducted in an open beaker. We believe that this was due to the differences between the power supplies used in two experiments. 3. Discussion Favarque et al. report observing COP's up to 1.4 in their experiments. Similar values were observed by other researchers. Clearly we have not replicated such results. How can this be explained? By experimental errors (measuring E, Qi, and Q2), or by unrecognized, but significant differences in experimental setups. Conditions under which experiments were performed might also have been different. Our anodes, for example, were made from platinized niobium while the anode used in Ref. 1 was made from platinized titanium. Instruments used to measure E were also very different. Accurate measurement of the electrical input power during plasma operation is complicated by the highly erratic current. In Texas, for example, the average current drawn by the cell was 2-3 A but the waveform peaks frequently exceeded 10 A. A sophisticated Clarke-Hess instrument was able to recognize overloads and signal them by flashing. On a less sophisticated instrument such conditions might be overlooked and will lead to underestimation of the average power being delivered to the cell. Overloads were observed during the initial testing; they were eliminated by placing a large filter capacitor between the Clarke-Hess instrument and the cell, as described in Ref. 8. Possible errors in measuring Qx and Q2 are discussed in Ref. 3.

173

Let us mention that appearances of the cathode glow discharge in Texas and in Colorado were quite different. In the first case, we occasionally observed white light flashes coming from large regions inside the cell, in the second only a steady yellow light was seen from a small region surrounding the cathode. Intense white light coming from large regions inside the electrolyte can also be seen on the Internet pictures of similar experiments performed by other researchers. Another difference worth mentioning was the fact that a typical current (for a given voltage) in Texas was about four times higher than in Colorado. The plasma differences between Texas and Colorado experiments were probably due to the arc suppression abilities of the Colorado power supply (see Appendix 1). Why is excess heat observed in some recent experimental s e t u p s 1 ' 5 - 7 and not in others? 8 Are the discrepancies due to experimental errors or to unrecognized, but essential, ingredients present in some setups and absent in others? It is difficult to answer such questions. Scientific disputes are not resolved by voting but a large number of confirmations of excess heat, by qualified researchers in many countries, should not be ignored. The existing controversy would be eliminated if a highly reliable portable excess heat generator could be built. Such generator would then be studied in different laboratories. How else can a consensus be reached? Referring to the issue Jed Rothwell9 wrote: "This is more art than science. Direct, hands-on learning may be the only way to grasp these things; Mizuno himself does not know what is going on in many ways. Building devices on the basis of described protocols does not seem to be sufficient." That is a very good point. A tentatively accepted theoretical model would certainly synchronize our efforts to make sense out of what is going on in the CMNS field. Trying to confirm or to refute claims made by individual researchers is certainly much less effective than testing various aspects of a tentatively accepted model. P.S. ( 1 2 / 2 / 0 5 , by Ludwik Kowalski) Unfortunately, one important detail, about the protocol used by Fauvarque et al, was not specified in Ref. 8. As I learned from Pierre Clauzon (at the ICCF12) the voltage applied to the cell must change gradually, typically in 20 V increments every minute or so. During that time, the cathode was said to be preconditioned to produce excess heat. Clauzon said that they also failed to confirm reality of excess heat without preconditioning. Appendix 1: Power Supply in Colorado Experiment The power supply used in Colorado was Pinnacle. 10 Although the supply was designed for other purposes, it seems to be ideal for glow discharge experiments. Its typical applications include dc sputtering with RF bias, basic magnetron sputtering, cathode-arc deposition (sputter etching and DC-biased RF sputtering). The special features of the Pinnacle are as follows: (1) High line to load efficiency 91%. (2) Power factor >0.9 for loads greater than 1.2 kW.

174

(3) (4) (5) (8) (9)

Quick response to changes in the load. Extremely low-stored energy in the output filter. Fast arc-suppression. Ability to preset joules to be delivered to the load. Provides up to 20 kW of continuous power (we did not exceed 2kW).

The supply provides very accurate power measurements and the ability to control how the power is delivered to the cell. Pinnacle can be used as a source of constant voltage, constant current, or constant power, depending on what is chosen. The other two parameters are then determined by the load. The output voltage, current, or power will hold to within ± 1 % as long as the load impedance stays within the voltage and current limits of the unit. Our tests were performed by using the constant voltage mode, in the voltage range between 400 and 800. The low-stored energy of the output filters of the Pinnacle allows the regulation system of the supply to rapidly respond to changes in the cell impedance. The lowstored energy also prevents the supply from dumping large amounts of energy into the cell as its impedance changes. The low-stored energy is probably one reason that we did not experience the violent reactions in the electrolyte. The other reason was probably the built-in arc suppression. The pinnacle has several methods of arc suppression. The one we used is called "micro-arc suppression." When an arc of less than 10 (is occurs, the stored energy is diverted from the cell and the growing arc is extinguished. The voltage is restored, approximately 5 ^s later. This ability is used in industry to maintain steady even plasma that are required for precise deposition of material on the manufactured product. This arc suppression in combination with the low-stored output energy of the Pinnacle was most likely the reason that we were able to increase the potential difference to over 700 V without the violent reactions in the electrolyte. The arc suppression might also be a reason that our results are different from those reported in Ref. 1. According to Ref. 9, Mizuno says "anyone can generate plasma with hundreds of volts. The trick is to generate it and then gradually reduce input power to the minimum." In one of his papers he writes: "Some researchers have attempted to replicate the phenomenon, but it has been difficult for them to generate large excess heat. They have tended to increase voltage to a very high value, around several hundred volts, but they measured no excess heat." Mizuno also indicates that when the cell begins to produce excess heat the conditions inside the cell are placid. These are the same conditions that we observed in Colorado. We recognize that the cost of the Pinnacle would make it prohibitive for most experimenters. There are, however, less expensive techniques for arc suppression that could be added to power supplies. It is likely that arc suppression will help to minimize the power delivered to the cell, at a given voltage. This might be an important precondition for the generation of excess heat, as indicated by Mizuno.

175

Appendix 2: On Water Condensation Inside Cells A critical reader might notice that Fauvarque et al.1 used an open beaker while the cell used in Texas had a lid on top of it. Can this possibly be a reason for the discrepancy between the outcomes of the experiments? The fraction of steam condensing in a cell with a lid is certainly larger than in a nearly open cell. The rate at which the mass is lost is used in the calculation of COP. Therefore, a critical thinker might say, the difference in the reported values of COP is not surprising. This issue was discussed in Ref. 3. The conclusion was that no significant errors are expected from condensation of water inside the electrolyte, provided the non-evaporative losses are also measured, as in Ref. 1. But that was only a logical conclusion based on certain assumptions. Here is how the conclusion was experimentally validated in Colorado. (a) One liter of water was placed into a 21 beaker standing on a scale, as in Ref. 1. An ohmic heater was used to sustain boiling. The cell had no lid. The mass lost in 350 s was found to be 40.1 g. (b) The cell was then covered with a plastic plate. That plate had eight holes (about 1cm diameter each) plus a hole for the ohmic heater cable. The amount of water lost in 350 s turned out to be 26.1 g. This confirmed the obvious - condensation is enhanced by covering a cell. (c) A pair of plasma experiments was performed - one with a nearly open cell and another with a nearly covered cell. The calculated COP turned out to be 1.00 when the cell was closed (to prevent anticipated splashing that did not materialized) and 1.07 when the cell was essentially open. This pair of tests, by the way, was conducted at 700 V. Pairs of tests at 600 and 550 V also showed that the values of COP are nearly identical and very close to unity. Appendix 3: On Reporting Negative Results After finishing Colorado experiments, one of us (L.K.) called a friend and talked about the discrepancy between our results and results reported by other investigators of plasma electrolysis. This prompted him to write the following message: "I am a retired physics teacher interested in all three CMNS phenomena: CF (cold fusion), CT (cold transmutations), and EE (excess energy). We know that there are two kinds of experimental results: unreliable and reliable. Unreliable data are obtained when experiments are being set up and when we are not yet sure that things work properly. Once the initial difficulties are overcome researchers think that results are reliable. Suppose that reliable experimental data were obtained in 10 experiments. Two of these experiments confirmed the expectations and eight did not confirm them. How should such situation be handled? What should a scientific conference report contain, only two positive results or all results? I know that our natural tendency

176

is to focus on the most interesting new results. But is this appropriate? I do not think so. Negative results should not be confused with unreliable results ..." But the situation is complicated by the fact that some researchers might be hesitant to publish negative results. They might fear that negative statements, taken out of context, can be quoted by pathological skeptics criticizing the field. In our opinion, such fears are not justified; benefits from sharing all reliable results far outweigh negative consequences of self-imposed secrecy. Unscrupulous critics, such as Dr. Richard Park, should not be feared by honest researchers. The issue of publishing negative results goes to the heart of scientific methodology. Here is what Ed Storm wrote about publishing negative results (a private message, 11/19/05): "I would like to throw out some counter thoughts. I think publishing negative results is a waste of time unless these results reveal a useful pattern. For most phenomena, millions of ways are available that will fail to generate the desired results. In contrast, many fewer methods will give the desired results. When isolated negative results are reported, they provide no guidance because they are only a few of so many possible ways to fail. The negative results must be shown to relate to a pattern or a general characteristic. For example in CF, if the H2O content of the electrolyte is too high, the results will be negative over a wide range of concentration. Unless this fact is related to a positive result obtained when the H2O content is low, the observations have little value. My point is that people reporting negative results should be required to show an understanding of their meaning just as people reporting positive results must show what their results mean. However, this does not mean that negative results can be used to deny the possibility of positive results. The two kinds of results have very little relationship to each other until the positive results are well understood, because as I said at the start of these comments, many ways exist for a real result to fail." We do not agree with this. Negative results are worth sharing and discussing. In this report, for example, one of us (R.L.) speculated that our negative results might be associated with the absence of arcing (collecting data when arcing was not too intensive in Texas and suppressing arcing electronically in Clorado). Is it possible that arcing superimposed on the quite glow discharge is an essential component of a device generating excess heat? R.L. plans to answer this question experimentally in the near future. We think that negative results are worth sharing because, like positive results, they guide our attempts to understand what is going on. At one point, two of us (R.L. and L.K.) were discussing the magnificent Naudin's report: http://jlnlabs.imars.com/cfr/html/cfdatas.htm The scatter plot called "efficiency..." shows results from a large number of experiments that were similar to ours. We noticed that in all 22 experiments (performed at 200 V or above) the excess heat was larger than 20% of the input energy. That is a highly significant result; the voltage-dependence trend seems to be consistent with what was reported in Ref. 1. That is how the issue of "publishing positive results only" came about. Negative results were not mentioned. We assumed that

177 the impressive 22 d a t a points represent 100% of reliable experiments. But what if this were not true? We would be much less impressed if these 22 d a t a points represented only 30% of all reliable experiments. Negative results, if any, are important indications of encountered difficulties. P.S. Subsequently Ed wrote: "You may quote me and even use my name. However, your counter argument to my comment missed the point I was making. As I said, "I think publishing negative results is a waste of time unless these results reveal a useful pattern." T h e "useful pattern" is the important aspect of my comment. In your reply, you showed t h a t your negative results were being used to reveal a useful pattern, i.e. t h a t the nature of arcing was a possible important v a r i a b l e . . . During my present study of the F - P effect, I have had many "negative" results. However, I know t h a t certain variables are important and must be controlled. For example, no excess energy is possible unless the D / P d ratio in the surface is very high, which is a difficult condition to achieve. Therefore, I a m investigating the processes t h a t affect this composition. If I report all the negative results without relating t h e m to the important variables, I would be wasting everyone's time. References 1. J. Fauvarque, P. Clauzon, and G. Lalleve, Abnormal excess heat observed during Mizuno-type experiments. Laboratoire d'Electrochimie Industrielle, Conservatoire National des Arts et Metiers: Paris (2005). Available as: (http://www.lenrcanr.org/acrobat/FauvarqueJabnormalex.pdf) 2. See (http://www.earthtech.org/experiments/Inc-W/Fauvarque) 3. See (http://blake.montclair.edu/~kowalskil/cf/2671ittle.html) 4. See (http://blake.montclair.edu/~kowalskil/cf/270slaughter.html) 5. T. Mizuno, D. Chang, F. Sesftel, and Y. Aoki Generation of Heat and Products During Plasma Electrolysis, in Eleventh International Conference on Condensed Matter Nuclear Science, (Marseille, France, 2004). Downloadable from the library at (http://www.lenr-canr.org) 6. D. Cirillo, A. Dattilo, and V. Iorio, Transmutation of metal to low energy in confined plasma in the water (electrochemical plasma cell), in Eleventh International Conference on Condensed Matter Nuclear Science (Marseille, France, 2004). Downloadable from the library at (http://www.lenr-canr.org) 7. Jean-Louis, Naudin et al. Several illustrations and references are downloadable from (http://jlnlabs.imars.com/cfr/index.htm) and from (http://jlnlabs.imars.com/ cfr/html/ cfrtpwr.htm) 8. Scott R. Little, H.E. Puthoff, and Marissa E. Little, Search for excess heat from Pt electrolyte discharge in K2C03-H20 and K2C03-D20 electrolysis. Downloadable from (http://www.earthtech.org/experiments/Inc-W/Mizuno.html) 9. Jed Rothwell, private communication (November, 2005). 10. The Advanced Energy Industry Inc, Fort Collins, Colorado, 80525 (http://www.advanced-energy.com/upload/Pinnacle%20Series%20DC% 20Magnetron%20Power%20Supplies.pdf)

OBSERVATION OF SURFACE D I S T R I B U T I O N OF P R O D U C T S B Y X-RAY FLUORESCENCE S P E C T R O M E T R Y D U R I N G D2 GAS P E R M E A T I O N T H R O U G H Pd COMPLEXES

YASUHIRO IWAMURA, TAKEHIKO ITOH, MITSURU SAKANO, NORIKO YAMAZAKI AND SHIZUMA KURIBAYASHI Advanced

Technology Research Center, Mitsubishi Heavy Industries 1-8-1 Kanazawa-ku, Yokohama 236-8515, Japan E-mail: [email protected]

Ltd.,

YASUKO TERADA Japan Synchrotron

Radiation

Research Institute, Hyogo 679-5148,

1-1-1 Kouto, Japan

Sayo-cho,

Sayo-gun,

T E T S U Y A ISHIKAWA Coherent

X-Ray

Optics Laboratory, Sayo-gun,

RIKEN Harima Institute, Hyogo 679-5148, Japan

1-1-1 Kouto,

Sayo-cho,

In-situ measurement of transmutation of Cs into Pr was performed, and the surface distribution of Pr was investigated using X-ray fluorescence spectrometry (XRF) at SPring-8, a large synchrotron X-ray facility. The in-situ measurement indicated that Pr emerged and Cs decreased at some points after Di gas permeation, though any Pr cannot be observed before Z>2 gas permeation at all the points on the Pd complex surface. Using small size X-ray beam in 100- and 500-fim 2 , we obtained two-dimensional XRF spectra for three permeated samples, from which we detected Pr. Pr was detected again by the two small X-ray beams as expected. The amount of Pr varied greatly at different locations of the Pd surface, however, a clear correlation between surface structures and distribution of Pr has not seen up to now. Experimental results suggest that nuclear transmutations do not occur uniformly but some uncertain factors, presumably condensed matter effects in the present P d / D / C a O system, have a large effect on the rate or the process of the reactions.

1. Introduction Low-energy nuclear transmutations in condensed matter have been observed in Pd complexes which are composed of Pd and CaO thin film and Pd substrate, induced by £>2 gas permeation through Pd multilayer complexes. We already reported transmutation reactions of Cs into Pr, Ba into Sm and Sr into Mo, respectively.1_5 Figure 1 shows schematic of our method. Our experimental method can be characterized by the permeation of D2 gas through the Pd complex and the addition of an element that is specifically targeted to be transmuted. Permeation of deuterium is attained by exposing one side of the Pd complex to D2 gas while maintaining 178

179

the other side under vacuum conditions. On the D 2 gas side of the Pd complex, dissociative absorption causes the D 2 molecules to separate into D atoms, which diffuse through the Pd metal toward the vacuum side, where they emerge from the Pd metal, combine and are released as D 2 gas.

D permeation

^ i ^

^ j ^

^l^

ii

Cs, Ba, etc.

t i I

D flux

I

Vacuum

Figure 1.

/i

i 1

Schematic of our experimental approach.

The second feature is the addition of an element targeted to be transmuted. Our sample is a Pd complex composed of bulk Pd on the bottom, alternating CaO and Pd layers, and a Pd thin film on top. After fabricating a Pd complex, Cs, Ba, Sr, or the other element is deposited on the surface of the top thin Pd layer. We can observe transmutation of the added Cs or Ba. In other words, with this composition, we can provide a deuterium flux through the Pd complex on which a target element is placed as a target to be transmuted. We perform elemental analyses of the given elements after D 2 gas permeation by exhausting the D 2 chamber. In this paper, in-situ measurement of transmutation of Cs into Pr and surface distribution are described. X-ray fluorescence spectrometry at SPring-8 (http://www.spring8.or.Jp/e/) was used for this study. Transmutation reactions of Cs into Pr were confirmed by the in-situ measurement. Surface Pr distribution data were obtained and they showed that the amount of Pr changed greatly depending on the locations of the Pd surface. 2. E x p e r i m e n t a l Fabrication of Pd complex is basically the same as before. 1-5 A Pd was washed with acetone and annealed in vacuum ( 23 Na Ne ->24 Na - 24 Mg 39 3 9 g _ > CI -+ 39 Ar 59 Cr -V^Mn - 5 9 Fe --. 5 9 Co 67 Ni- ^ 7 Cu --+ 67 Zn 69 Ni- -^69 Cu --^69 Zn -^69 G a ^ 6 9 G e 73 Zn -^ 73 Ga - 7 3 G e 81 Ga ^ 8 1 G e ^ 8 1 As --.81 g e ^ 8 1 B r 83 Ge ^ 8 3 As -- 8 3 Se -^83 B r ^ 8 3 K r 84 As- - 8 4 Se -^ 8 4 Br -H• 8 4 K r 87 As- - 8 7 Se --+87 Br -,87 fo ^ 8 7 R b 9 3 B r .- 9 3 Kr -^ 9 3 Rb -^93 g r ^ 9 3 Y ^ 9 3 & 94 Kr ^ 9 4 Rb ^ 9 4 Sr -4 94 Y ^ 9 4 ^ j . 99 Rb - + " Sr -_^99 y _> 99 Zr ^ " Nb - > " Mo 100y ^ 1 0 ° Zr ^ 1 0 ° Nb ^ 1 0 ° Mo 101y ^ 1 0 1 Zr -^ 1 0 1 Nb _ ^ i o i M o ^ i o i T c ^ i 2 4 p _ ,2i

105Nb ^105 115

Rh ^

115

M Q

^105

Pd ^

115

T(,

^105

Ag -^

115

R u

^105

Cd -^

115

R h

^105 p

d

In

The cathodes made of the different materials showed the value of inductive gamma-radiation after the GD current switch off. The intensity of the emission increased with the increase in dose of plasma ion radiation (D2, H2, Ar, and Xe) of the plasma forming gas for the cathode sample. The spectra of inductive gammaactivity include areas exceeding the continuous spectra (continuum) and the lines imposed on them. In this case the value exceeding the area of gamma line over

223 A/j

1 %

d

•

i" !

400

i i i

I I

600

/'

'f fk

200 W L & H - T A .1. 1

-Je.

-, 1

0

200

IW!^KH , &'MS ^ M *

600

400

800 E(keV)

Figure 7. Gamma emission spectrum recorded by Ge-Li detector from the GD device after, the discharge current switch off. Pd cathode placed in D2 discharge. The part of the spectrum area ("d" - area) is presented in greater detail (see Fig. 8.).

background (a) is not a large factor a (a = 2.5-5). The value for the continuum is a = 8-10. The gamma spectra obtained during the GD operation and after the GD current switch off were processed with the help of a database to identify gamma lines of radioactive nuclides.2 For each /^-transition 30 or 40 gamma lines were identified. For a single /3-radioactive decay chain (one atomic mass of radioactive nuclides) 100-200 gamma-lines were identified. The gamma emission spectrum registered after the GD current switch off contains gamma lines of short-lived (3- radioactive chains (Figs. 7 and 8). Presumably after the GD current switch off there appear certain conditions for initiating nuclear reactions. The total number of radioactive atoms was determined taking into account the values of gamma-line areas, the value of the detector efficiency, and the ,1

Ru, 306.8 'Br, 334.0 E E aaSr, 307.0 , , , — m,n 336 2 2% i«Tc, 309.5, ' -MO,

250

42

Ca^312.6

12,

200

107

^Rh, 374.3 374.9

101Tc, 408.7 84 Br, 408.2 105 Rh, 407.6

r

!3

Na, 440.0 Zn, 438.6

i9

Cd, 481.0 'Cd, 478.7

348.5 ' " N b , 373.9

Pd, 348.2

r°lNb

83

ln, 313.7 I

150 100 50

a

Br, 345.2 Pd, 344.5 115 Ag, 342.7

105

300

400

E, (keV)51

Figure 8. Part of gamma emission spectrum indicating identified gamma-lines The duration of the discharge operation was 10,000 s. The duration of the gamma spectrum registration was 60,000 s after the discharge current switch off. The background spectrum (60,000 s duration) was subtracted from the operational spectrum. The lines are identified as related to excited nuclei of beta-decay chains.

224

value of the quantum yield. The /3-radioactive chains with masses of A = 23, 24, 39, 59, 67, 69, 73, 81, 83, 84, 87, 93, 94, 99, 100, 101, 105, and 115, make the main contribution into gamma-radiation (operating time for radioactive nuclides is up to 10 5 atoms). 5. X-ray Emmission Registration The initial excitation energy up to several keV is needed to trigger the assumed nuclear reactions within the cathode sample solid (the density of the interactive nuclei corresponding to that of the solid). The existence of such excited energetic levels is evidenced by intensive X-ray emission from the cathode sample solid medium observed in the experiments. The recording of the X-rays was carried out using thermo-luminescent detectors (TLD), an X-ray film and scintillator detectors with photomultipliers. l The high intensity of the X-rays made it possible to obtain an optic image of the emission area. This was done by a pinhole camera (with 2.0 mm diameter hole as an optic lens). The image shows that the cathode area measuring 9 mm diameter (Fig. 9) and especially its central part is the most luminescent. The pinhole provided a spatial resolution of the X-ray emission. The X-ray emission registration by the pinhole was performed without any induced magnetic field, and, with lateral 0.3 T magnetic field induced in front of the pinhole (to deflect the charged particles flow from the cathode). Absence of noticeable difference between the two images (Fig. 9b and c) shows that the pinhole recorded the X-ray emission.

Figure 9. The diagram of the X-ray image registration using the pinhole. The objective with 2.0 mm diameter closes by the 15(im Be shield. The system Pd-D2, the discharge current: 150 mA; voltage is 1850 V; the exposure time: 10,000 s. (a) X-ray image registration without superimposition of the cross magnetic field; (b) X-ray image registration with superimposition of the cross magnetic field 0.3 T. The image is positive. (1) anode, (2) discharge plasma area, and (3) cathode.

The evaluation of the X-ray emission was made with reference to the change in the radiation dose absorbed by thermo-luminescent detectors covered with Be foils of varying thickness. The experimentally determined value of the X-ray energy increased from 1.2 to 1.5 keV when the thickness of the Be shield increased from

225 Table 7. The characteristic of X-ray emission from different cathode samples in Glow Discharge experiment. Material of cathode Glow discharge voltage (V) Glow discharge current (mA) X-ray energy during passing the discharge current, J3x—ray (keV) X-ray energy without current, J^X-ray (keV)

Al Sc Ti Ni 1650 1540 1730 1650 130 130 170 150 1.54 1.26 1.45 1.91

Mo Pd Ta Re 1420 1650 1600 1520 210 138 138 125 1.48 1.98 1.62 1.36

Pt Pb 1650 1610 138 138 1.47 1.36

1.68

1.33

1.75

1.5

1.46

1.96

1.71

1.62

1.38

1.45

15 to 300 /jm. X-ray emission as a function of time was studied with scintillator detectors and photomultipliers (PM). For different cathode materials the X-ray energy values obtained with the help of scintillator detectors, PM and 15 and 30 /iin-thick beryllium foils amounted to Ex-ra,y ~ 1.0-2.5 keV (Table 7), which showed good agreement with the TLD data. The X-ray spectra were determined using the curved mica crystal X-ray spectrometer fixed (positioned) on an X-ray film (Fig. 10). The X-ray wave length was evaluated by the expression: m x A = 2 x d x sin#, where A is the wave length, d stands for the distance between crystallographic planes of the mica crystal, 2 x d = 2nm; 9 represents Bragg divergence (angle); m stands for the diffraction order. The spectrum was registered both as bands of the continuum with energies ranging 0.6-10.0 keV and as spots resulting from the emission of series of high-density mono-energetic X-ray beams (with energies up to 0.6-10.0 keV) characterized by small angular divergence. The energetic position within the spectrum depended upon the cathode material used (was specific for a given cathode material) and was similar to characteristic X-ray spectra. Of particular interest was the persistence of the X-ray spectrum registration for several hours after turning off the GD current. Presumably, some long-lived excited levels with energies up to several keV are formed in the cathode solid-state medium, and after the GD current is cut off, the excitation persists maintained by the X-ray emission. The spectrum band ranging in energy 1.2-1.3 keV was defined for Pd cathode samples in D2 and Kr GD (during its operation, and after, the discharge current switch off) (Fig. 10). This result is in good agreement with the maximum value of excess heat power at 1000-1300 V GD voltage. 6. Discussion Experiments on anomalies in high-current glow discharge carried out for several years allow to outline the basic processes and conditions of their occurrence. (1) Excess heat production. Excess heat was produced in the volume of the solid-state medium of the cathode sample under the following conditions: • Deuterium should be loaded into the solid-state cathode medium.

226

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^ ? # ^ r : < r : . ; r •; • „ "#.,

20 10

5 0 40

:io

2.0

18

15

v

20 10

5.0 4.0

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v

Pd_Kr

Pd-Xe

* -\ 3.6 " "'

20

18

16

1.4

- ^ ^Tgrggjgip

?0 10

5 0 4.0

3.0

2.0

1.8

1.6

1.4

^x-ray (keV)

Figure 10. The outline of X-ray spectrum registration from the Pd cathode sample using the curved mica crystal spectrometer. (a5 b, c, d) during the GD operation, the exposure time is 18,000 s. (a) during the GD operation in D2; (b, c, d) the Pd cathode samples are non deuteriumcharged, (b) GD in Ar, (c) GD in Kr, (d) GD in Xe, (e) the spectrum registered after the GD in D2 current switch off.

® Initiating excitation of the energy levels of the crystal lattice of the cathode material was necessary. ® This initiation could be achieved by a foreign source (e.g., by a flow of inert gas ions). ® The production of the excess heat power occurred mainly in the nearsurface layer of the cathode sample with the thickness up to 1/im (where the impurity nuclides were found). The volume density of the excess heat power showed a value up to 105 W/cm 3 . (2) Production of elements (isotopes) as an induced impurity of the basic cathode material.

227

• The production of impurity nuclides occurred in the volume of the solid-state cathode medium, presumably, as a result of nuclear transmutation reactions. • The emission of high-energy heavy ions was not recorded in the experiment. This allows to assume, that the nuclear reactions energy was not released as a kinetic energy of the formed impurity nuclides. The impurity nuclides may be assumed to form as nuclear isomers (the nuclei being in the excited state). The results of the experiment showed that the relaxation of these excited nuclear levels through the gammaradiation channel was strongly suppressed. (3) Excitation of the energy levels in the solid-state cathode medium. • Formation of the excited energy levels in the crystal lattice was evidenced by recording the X-rays from solid-state cathode. • X-rays were observed as bursts of short duration (presumably up to 1 0 - 1 3 s). Each burst contained up to 109 X-ray quanta with the energy of 1.5-1.8 keV. The bursts were recorded in amount of up to 105 bursts per second during the GD operation and within 100 ms after turning off the GD current. • Hypothetically, the mechanism of forming this radiation was the following. When bombarding the cathode surface by the discharge plasma ions in the solid medium, excited energy levels with the energy of 1.5-2.5 keV and lifetime up to 100 ms were formed. Looking into the concrete physical mechanism of forming these levels requires some additional research. It is possible to assume the existence of one of the two possible physical phenomena: (1) excitation of internal electronic - nuclear system without ionizing the external electrons; (2) oscillatory deformation of the electron-nuclear system of the solid ions. The core of electronic shells was displaced from a nucleus with forming a dipole (optical polar phonon). • The relaxation of the excited energy levels of the solid medium occurred through the emission of X-rays and, perhaps, fast electrons. • Hypothetically, the relaxation of the excited levels occurred simultaneously from micro mono-crystals that make up the solid medium. In other words, the totality of the excited ions of the micro mono-crystal relaxed simultaneously and gave the X-rays burst. (4) Nuclear transmutation reactions. The excited energy states with the population density of n ex ; t (cm - 3 ) and a characteristic temperature of Texit ~ 1-5-1.8keV, and more (up to 20,000,000 K, and more), were formed in the solid with every pulse of the glow discharge current. These energy states existed for the characteristic time Texit (up to 100 ms and more). Such medium, in which the temperature of the crystalline lattice did not exceed some hundreds Kelvin, we call a non-equilibrium medium.

• Occurrence of non-equilibrium nuclear transmutation reactions was made possible in such medium. Probability of running these reactions (and accordingly the value of the excess heat power) was determined by the criterion: ^exit X T ex it /* (^exit -* T e x itjmiii'

This criterion was a modified Lawson's criterion used for estimating the positive heat output at inertial thermonuclear synthesis. • The population density was defined by the parameters of the discharge duration and the cathode sample geometry. The characteristic lifetime of the excited states was defined by the balance between the processes that produce excitation of the energy levels (when passing a pulse of the pumping discharge current), and, relaxation processes of these levels (by emitting the X-rays). Thus, for obtaining large quantities of the excess heat power it was necessary to create a high population density of vibration- dipole energy states n ex it and to suppress the X-rays emission (for increasing a lifetime of the excited states Tex;t). (5) The following types of the nuclear transmutation reactions resulting in formation of the stable nuclides are possible: A + m B ^ [AB]*, A + A + m B ^ [2AB]*, [AB]* - ^ F * - ^ F + Heat, [AB]* -> C * +D* - • C + D + Heat, where A is Pd or the nucleus of another element; B stands for deuterium or hydrogen; [AB]* represents short-lived intermediate compound nucleus; m = 1, 2, 3 , . . . , C*, D* are the nuclear isomers of nuclides with masses less than that of Pd; C,D are stable nuclides, F stands for a nuclide with mass more than that of Pd. First a composite compound-nucleus in the excited state is formed. Then one of the two possible modes is realized: (a) The compound-nucleus could lose its excitation and form a stable nucleus, being heavier than Pd; (b) the compound nucleus could fission into two nuclear fragments with masses less than that of Pd. In doing so, the two nuclei should be in excited isomeric states (experiments showed that the nuclear reactions energy was not produced as a kinetic energy). (6) To determine the specific physical mechanism for these reactions requires some additional research. One possible type of reaction for forming the impurity nuclides can be long-range (resonant) nuclear reactions. The mechanism of such long-range reactions can be explained using as an example a specific transmutation reaction for Pd + D (Fig. 11a) and Pd + 2D (Fig. l i b ) .

229

The formation of significant 13 C nuclide and 93 Nb was recorded in the experiments. Assumedly, the reaction can proceed in the following way. 104

Pd+2D

[Pd;D]n

.13

C

93

Nb +7.820 MeV.

According to the laws of momentum and energy conservation, the formed nuclide 13 C should receive the energy of 6.8609 MeV. The nuclide 93 Nb should receive the energy of 0.959 MeV. The nuclear excited state (nuclear isomer) with the energy of 6.864 MeV and excited level width of 6 keV exists for 1 3 C. The excited level with the energy of 0.94983 MeV exists for 93 Nb. The difference between the energy received by nuclide 13 C and the energy of one of the excited nucleus equals to 3.f keV. At the excitation energy of the crystalline lattice of 1.5 keV, and width of the excited energy level of 6.0 keV, these conditions resulted in a high probability for occurrence of the long-range (resonant) nuclear reaction. 105

Pd + 2 2 D - • [Pd2D]* -^ 9 3 Rh + b Li + 11.794 MeV.

According to the laws of momentum and energy conservation, the formed nuclide Li should receive the energy of 8.880 MeV. The nuclide 93 Nb should receive the energy of 0.959 MeV. The nuclear excited state (nuclear isomer) with the energy of 6.864 MeV and excited level width of 6 keV exists for 1 3 C. The excited level with the energy of 0.94983 MeV exists for 93 Nb. The difference between the energy received by nuclide 13 C and the energy of one of the excited nucleus equals to 3.1 keV. 6

. = 7820 keV

11794keV

5a

~

HiLi*ex.lev. 6Lin.r

fc

13Cn.r

r^j I >

3.1

CD

n Ul

^




CD O

+

686

rt

1 93

I

5/2

CD

ev.

13

'

C stable

[Pd2D]*

103

Rh stable

6

Li stable

Figure 11. Assumed plan of carrying out long-ranged (resonant) nuclear reactions, (a) for Pd D transmutation reaction and (b) for Pd + 2D transmutation reaction.

The totality of the experimental results allows to assume that the energy of the excited nuclear levels of the formed nuclides converts into heat. The specific physical mechanism of such conversion requires additional research.

230

7.

Conclusions

T h e results obtained (the glow discharge device producing the excess heat power up to 5 W / c m 2 at an efficiency up to 150%) allow the development of a demonstration source of heat power. The technology for development of multi-element cathode fuel elements with plasma anodes has been worked out. The development of new nuclear engineering is possible based on non-equilibrium nuclear t r a n s m u t a t i o n reactions in the solid-state medium. This type of engineering can be called "Third way" in nuclear engineering in comparison with the nuclear engineering based on uranium nuclear fission, and thermonuclear synthesis.

References 1. A.B. Karabut, Ya.R. Kucherov, and I.V. Savvanimova, Nuclear product ratio for glow discharge in deuterium, Phys. Lett. A, 170, 265, 1992. 2. Richard B. Firestone, Table of Isotopes, 8th Edition, Vols. 1 and 2, Appendix G - 1 , John Wiley & Sons, Inc., New York, 1996.

I N F L U E N C E OF P A R A M E T E R S OF T H E GLOW D I S C H A R G E ON C H A N G E OF S T R U C T U R E A N D T H E ISOTOPE COMPOSITION OF THE CATHODE MATERIALS

L B . SAVVATIMOVA A N D D.V. G A V R I T E N K O V Federal State Unitarian Enterprise Scientific Research Institute "Luch", Zheleznodorozhnaya, 24 Podolsk, Moscow region 142116, Russia E-mail: [email protected]

Results of examinations of changes in structure, element, and isotope composition of cathodes after the glow discharge exposure in hydrogen, deuterium, argon, and xenon are submitted. The voltage of the discharge was less than 1000 V and the current was 5-150 mA. Samples before and after ions bombardment in the glow discharge were explored by the methods of mass spectrometry: the secondary ions (SIMS), the secondary ions with additional ionization of neutral sprayed particles (SNMS), spark (SMS), and thermo-ionization (TIMS), and also methods of energy dispersion X-ray spectral analysis (EDX). The alpha-, beta-, gamma- emission, and gamma- spectrometry for radioactive uranium specimens were also carried out before and after experiments in the glow discharge. Changes in structure, isotope, and element composition of the cathode samples depend on current density, integrated ions flow (fiuence of ions), kind of irradiating ions and other experimental conditions. Attempts are made to estimate qualitatively and quantitatively the role of each of the parameters on intensity of the observed changes in cathode composition. It is shown that the maximum changes in structure, chemical and isotope composition of the cathode material occur in "hot points," such as craters from microexplosions, phase segregations, blisters and other new formations. Various methods of the analysis revealed that the basic elements Mg, O, Si, Al, and Ca with quantities up to per cents and more were prevailing in these zones and not found out before experiment. The greatest changes of the isotope relations were observed for iron, calcium, silicon, chromium after experiments with pulsing current. EDX method finds out the elements missing in the samples before experiment such as cadmium, strontium, tin. The isotopes with mass number 59 (Co 100%), 55 (Mn 100%), 45 (Sc 100%) are also not found in initial samples and background measurement by TIMS method. Results of changes in the element and isotope composition, which are found by various methods of the analysis, are compared with possible reactions of fusion-fission. It is noted that under different experimental conditions on various cathode materials similar groups of prevailing elements are find by various methods of the analysis.

1. Introduction As is known, the ionic processing of materials results in changing surface properties. It has been shown earlier that physical-mechanical properties, element, and isotope compositions in plasma of a glow discharge change. 1_9 The majority of the "additional" elements found after ion irradiation and not found before irradiation is distributed at the boundaries of grains 1 and in 231

232

local spots. 3 ' 4,9 They make up from the 10th fractions of a percent up to several percents. Thus in initial samples the content of separate impurity elements did not exceed 10~ 3 -10~ 4 at.% and EDX analysis could not reveal it. Groups of such elements as Sc, Ti, V, Ag, Cd, In, P, CI, Br, Ge, As, Kr, Sr, Y, Ru, and Xe have been found in Pd after irradiation by ions of all the types (D, H, Ar, and Ar+Xe), but in various quantities. 2 Elements with atom numbers Z = 26-31 (Fe, Cu, Zn, and Ga) were observed by the method of energy-dispersion X-ray spectral analysis (EDX) preferentially after irradiation by deuterium ions. As a result of EDX and radiography, it was supposed that nuclear transmutations occur more intensively on local sites. 1 - 4 Distinctions in the characteristic spectrums corresponding to various combinations confirmed the nuclear processes in local zones. 3 ' 9 Considerable changes of the isotope relations were observed for 10 B / n B , 1 2 C/ 1 3 C, 6 0 Ni/ 6 1 Ni/ 6 2 , 4 0 Ca/ 4 4 Ca, and 9 0 Zr/ 9 1 Zr. 3 Change of the isotope relation in i 09 / 107 Ag from 3/1 up to 9/1 was observed in different series of experiments. 3 ' 9 In this paper, the changes of structure, element, and isotope composition of palladium for various parameters of the discharge are compared. The role of the current sort in transmutation intensity is shown. The possible types of nuclear reactions for pairs of the elements observed in the cathodes after experiments are shown. 2. Methods of the Analysis and Parameters of Glow Discharge The installation had a vacuum discharge chamber with a cathode and an anode. The chamber was evacuated up to 10~ 2 Torr, and then it was filled by working gas up to 3 10 Torr. Deuterium, hydrogen, argon, and xenon were used as working gases. Samples were irradiated by currents with density of ~10-50mA/cm 2 and at discharge voltage of 50-1200 V. The discharge burning exposure was 1-40 h, diameter of samples ~20mm, thickness ^100 /xm, the irradiated area - about 1 cm 2 . Multilayer cathodes consisting of several foils approximately 100 /jm thick each for acquisition of data on change of the element and isotope composition on depth were used. The examinations procedure in detail is described in Refs. 3 and 9. The measurement system allowed recording current, discharge voltage, gas pressure, sample temperature, temperature of the inlet, output of the cooling water in the cathode, anode, and cooling jacket. Changes in the element and isotope composition were analyzed by EDX methods and mass spectrometry. The element composition of the cathode materials was studied on scanning electronic microscope Hitachi S-840 with Link Analytical LS - 5 for a spectral analysis, later the structure of the surface and the sample composition were studied by electronic microscope JEOL JSM 6460-LV using INCA for X-ray spectral analysis. The content of elements was estimated using programs INCA (Version 4.02). Time of the spectra recording is 2 min. The accelerating voltage of 10 kV for the analysis of lighter elements and 30 kV for heavier elements were used. The analyzed zone size was about 1 /im 2 for the probe analysis in point, and when scanning on the area it was up to ^250 x 200 /im 2 . Sensitivity of the method

233

was ~ 1 0 - 2 atom.%. Depth of an analyzed layer made up about 1 /xk. Elements 0 , F, S, Na, Mg, Al, Ti, Cr, and Fe are analyzed on Ka, Mo and Br - on La, W - on Ma of characteristic spectrums lines. Concentration of the ("additional") impurity elements was determined using the majority of main lines of the characteristic X-ray spectrum. Initial samples and samples after experiments in deuterium glow discharge are analyzed. Places with structural defects and new formations such as swellings (blisters), craters, areas of micromeltings, needle structures, and sites of surface without special changes after irradiation in glow discharge plasma were explored. The isotope composition of the samples at high temperature was determined by the method of the thermo-ionization mass spectrometry on mass spectrometer "Finnigan"-262. The sample temperature in this analysis usually exceeded 1800°C. The majority of complex compounds should break up (dissociate) at such a temperature while the secondary ionic mass spectrometry can give many composite complexes. 3. Changes in Structure of Surface, Element, and Isotope Composition It is shown that changes of structure, element, and isotope composition depend on the following: (a) (b) (c) (d) (e)

Doses of irradiating ions (Tables 1-3).1 Density of ions current (Tables 4 and 5). 3 ' 4 Irradiating ions kind (Tables 4 and 5). 3 ^ 5 Current sorts: direct or pulsing (Tables 6, 12, and 13). Places of "hot points" analysis and new formation (Tables 8-12).

Each of the above process parameters (a-d) influenced on the process intensity and its reproducibility. The role of "hot points" in the change of structure, chemical, and isotope composition3-"5 and the groups of the elements dominating in these "active sites" are analyzed by various methods. 1 ' 2 ' 5 In this paper special attention is paid to structural change in new formations (in zones of craters, growth formations, and blisters) and to the effect of current (direct and pulsing). 3.1. Dependence

of "Additional"

Elements

Quantity

on Dose

Changes of the isotope and element composition of the samples irradiated by deuterium ions after different exposure time (dose) were analyzed by several methods. Table 1 comprised the data received by method of secondary ionic mass spectrometry after 30 min bombarding of palladium by deuterium. Table 2 includes the results of EDX data, and Table 3 has the same samples data obtained by method of spark mass spectrometry. The increase in the content of Li (Table 1) by a factor of 50-450 (rows 1 and 2), n B by a factor of 70 (row 4) can be a result of nuclear process under conditions

234

of low-energy actions in glow discharge plasma with the participation, for example, of hydrogen or deuterium, or processes of heavier elements fission. The increase in the content of Zr by a factor of after P d / P d critical electrolysis with current density of 3.6 A / c m 2 , for 10days in I M K2CO3 solution. Magnifying power and scale standard line are shown at the bottom of each photograph. The craters whose maximum size is over 10 fim. are located along the surface cracks.

261

On the cathode surfaces the countless Ohmori-type palladium craters were observed as an indirect evidence of nuclear reactions. These craters, which are located along the surface cracks or grain boundaries, were observed on the cathode only up until now. This result indicates that the nuclear reactions occur more easily around the surface and the cracks. The maximum width and height of craters are over 10 /mi. These crater sizes have a positive correlation with the current density. This result supports our prediction that the amount of excess heat and transmutation have a positive correlation with increase of current density. Therefore, the critical region is optimum to induce the nuclear reactions as described above. 4.4.

Discussion

To our knowledge, this is the first report of the Ohmori-type craters observed on the palladium electrodes. The characteristics of these palladium craters are similar to the gold craters first reported by Ohmori et al.3 Although the report was made 10 years ago, the formation mechanism is still unknown. Kamada et al. reported anomalous heat evolution and surface melting of deuteron implanted aluminum foil upon electron bombardment. 17 They estimated that the amount of anomalous heat exceeds the total amount of any kind of chemical reactions and, therefore, concluded a novel nuclear reaction had been occurred in the deuterated aluminum. If palladium electrode were melted due to this type of nuclear reaction, the palladium gas should be erupted. Then it should have cooled down in the solution to be recrystallized like the crater. Numata et al. found vortex patterns on well annealed thick palladium electrodes after a long-term heavy water electrolysis,18 and simulated a magnetic interaction of hypothetical particles to elucidate an evolution mechanism of vortexes. 19 They showed the vortex can be formed at the electrode/electrolyte interface by FEM method. If charged palladium particles dissolved from the anode were caught in a vortex, which is generated at the electrode/electrolyte interface, they might be accumulated to the cylindrical shape like the vortex to form the craters. Mizuno et al. described a large explosion that occurred during a normal light water electrolysis. 20,21 They made a rough estimate of the energy balance and concluded that it could not be a simple explosion, but rather it must have been caused by a large burst of anomalous heat. If micro explosions occurred on the electrode surface from this same type of heat, craters could be generated. It is still difficult to explain the mechanism by these theories. Although they may be impurities electrodeposited uniformly, we claim that the crater is an indirect evidence of nuclear reaction occurred at the electrode surface. 5. Conclusion P d / P d light water critical electrolyses were performed as the optimum condition and system to induce nuclear reactions. In this study the shape of both electrodes

262

was just same and the current density was over 2.5 A / c m 2 , for 7 or 10days, in 1 M K2CO3 solution whose t e m p e r a t u r e was u p to 70-90°C. After the experiment, the obvious t r a n s m u t a t i o n products namely iron, titanium, chromium, manganese, and nickel were detected by EDX. In particular, the iron peaks are very strong and detected from all cathode samples. The anomalous isotopic yield of detected iron should be expected since the anomaly has already claimed by many researchers. 3 ' 4 ' 2 2 T h e elements detected from the b o t h electrodes, namely, copper, zinc, and magnesium, however, cannot indicate their origin at this time. If they are t r a n s m u t a t i o n products, at least two mechanisms exist. T h e analysis of isotopic yields for all elements detected by SIMS must be indispensable to prove nuclear reactions. Quantitative analysis of the detected elements, distribution especially around craters, and isotopic yields are under considerations. Moreover, nuclear radiation detection could give important information to evaluate the process. Precise heat measurement is also required. Accurate estimation and reduction of impurities is also vital. Although the isotopic yields have not confirmed yet in this study, Ohmori et al. have already reported anomalous isotopic distribution of palladium with excess heat in their P d / P t critical electrolysis s y s t e m . 7 , 8 Furthermore the indirect evidence of nuclear reactions, namely Ohmori-type palladium craters were observed for the first time. Since the t r a n s m u t a t i o n products and the surface damages have been found, P d / P d critical electrolysis is optimum to induce condensed m a t t e r nuclear reactions. References 1. 2. 3. 4. 5. 6. 7. 8. 9. 10. 11. 12. 13. 14. 15. 16. 17.

T. Ohmori and M. Enyo, Proc. ICCF4 1, N2.3 (1993). T. Ohmori and M. Enyo, J. New Energy 1(1), 15 (1996). T. Ohmori, T. Mizuno, and M. Enyo, J. New Energy 1(15), 90 (1996). T. Ohmori, M. Enyo, T. Mizuno, Y. Nodasaka, and H. Minagawa, Fusion Technol. 31, 210 (1997). Y. Toriyabe, T. Mizuno, T. Ohmori, and Y. Aoki, Proc. JCF6 11 (2005). T. Mizuno, T. Ohmori, and T. Akimoto, Proc. ICCF10 (2003). T. Ohmori, S. Narita, H. Yamada, T. Mizuno, and Y. Aoki, Proc. JCF4 22 (2003). T. Ohmori, T. Mizuno, H. Yamada, and S. Narita, Proc. JCF5 36 (2004). A. Takahashi, H. Numata, H. Yamada, Y. Iwamura, T. Ohmori, T. Mizuno, and T. Akimoto, Study Nucl. React. Solid 159 (1999). T. Ohmori, Curr. Top. Electrochemistry 7, 102 (2000). T. Mizuno, T. Ohmori, T. Akimoto, and A. Takahashi, Jpn. J. Appl. Phys. 39, 6055 (2000). T. Mizuno, T. Akimoto, K. Azumi, T. Ohmori, Y. Aoki, and A. Takahashi, Jpn. J. Appl. Phys. 44(1A), 396 (2005). T. Ohmori and T. Mizuno, Curr. Top. Electrochemistry 5, 37 (1997). M.C.H. McKubre, S. Crouch-Baker, A.M. Riley, S.I. Smedley, and F.L. Tanzella, Proc. ICCF3 5 (1993). K. Kunimatsu, N. Hasegawa, A. Kubota, N. Imai, M. Ishikawa, H. Akita, and Y. Tsuchida, Proc. ICCF3 31 (1993). A. Takahashi, M. Ohta, and T. Mizuno, Jpn. J. Appl. Phys. 40, 7031 (2001). K. Kamada, H. Kinoshita, and H. Takahashi, Jpn. J. Appl. Phys. 35, 738 (1996).

263

18. H. Numata, R, Takagi, I. Ohno, K. Kawamura, and S. Haruyama, Proc. ACCF2 71 (1991). 19. H. Numata and M. Ban, Proc. ICCF12 (2005). 20. T. Mizuno, Y. Toriyabe, A. Takahashi, and A. Takada, Proc. JCF6 19 (2005). 21. T. Mizuno and Y. Toriyabe, Proc. ICCF12 (2005). 22. G. H. Miley and J. A. Patterson, J. New Energy 1(3), 5 (1996).

P R O G R E S S O N T H E S T U D Y OF ISOTOPIC C O M P O S I T I O N IN METALLIC THIN FILMS U N D E R G O N E TO ELECTROCHEMICAL L O A D I N G OF H Y D R O G E N

M. A P I C E L L A A N D V. V I O L A N T E ENEA

Frascati Research

Center, V. le E. Fermi 45, 00044 Frascati E-mail: violante®frascati. enea.it

(Roma),

Italy

F . S A R T O , A. R O S A D A A N D E. S A N T O R O ENEA

Casaccia

Research

Center,

V. Anguillarese (Roma), Italy

301, 00060 S.Maria

di

Galeria

E. C A S T A G N A A N D C. SIBILIA La Sapienza

University,

Via Scarpa,

14, 00100 (Roma),

Italy

M. M C K U B R E A N D F . T A N Z E L L A SRI International,

333 Ravenswood

Ave, Menlo Park,

CA 94025,

USA

G. H U B L E R Naval Research

Laboratory,

4555 Overlook Ave.,

S.W.

Washington,

DC 20375,

A research activity has started some years ago in the framework of collaboration between the ENEA (Italy) and the SRI (USA), aimed to the identification of traces of nuclear reactions in condensed matter. This work has also involved cross-linked analysis in order to identify effects due to contaminants that could affect the isotopic shift estimate. Nickel thin films have been sputtered on a polymeric substrate and loaded with hydrogen by electrolysis. Reference and active thin films have been prepared contemporaneously during the same sputtering process to have on both the same deposition and the same impurities composition. Secondary Ion Mass Spectroscopy (SIMS) has been used to analyze the isotopic composition of the electrolyzed and blank substrates. Preliminary results (Violante et al, Proc. 10th Int. Conf. Cold Fusion (ICCF-10), Cambridge, 2003) indicated that a reasonable reproducible apparent shift of the isotopic composition of the Cu element occurred in some of the electrolyzed films, with an increasing of mass 65, while the natural value was always observed for all the blank samples. Cu was particularly suitable for being used as a marker elements because of its only two mass isotopes (63/65) that do not overlap with isotopes of other elements having the same masses. In this work, new experiments have been reproduced to increase the statitistics and further analysis has been performed in order to exclude that the revealed shift was traceable to an artifact.These included SIMS scanning of the sample surface, depth profile analysis by SIMS, mass spectrometric analysis of the electrolyte, SUPER-SIMS [2] analysis of one couple of reference and active films. In particular, the possible contribution from mass interferences on the 65-mass extrasignal has been considered, coming from contaminants or double ionized species. On the basis of the new results, a more complex scenario has been evidenced,

264

USA

265 suggesting that the former attribution of the C u 6 3 / C u 6 5 isotopic shift could be not correct. The indication of new experiments and tests that potentially should provide a complete understanding of the present results has been given. The work wants to stress that the identification of elemental transmutations in metal hydrides is an extremely complex topic, which necessitate of severe scientific accuracy, cross-matched analysis, multidisciplinary expertise, and the access to top performance experimental facilities. All these requirements can be fulfilled only in the framework of top-level international scientific collaboration.

1. Introduction The detection of nuclear ashes inside metallic hydrides is one of the most direct evidences of the happening of nuclear reaction in the condensed matter. But this topic is also a very complex and delicate issue, first of all because of the low level of the signals to be detected, which can be easily overlapped by instrumental noise or background interferences. The measurement of the isotopic composition of metallic hydrides is an efficient method to reveal nuclear products eventually formed during the hydrogen loading. Actually, the presence of "new" (i.e. "not detected before") elements in the metal specimens cannot be assessed as products of a nuclear reactions, because the possibility of contamination from the environment or the diffusion of impurities inside the sample to the detection areas are very difficult to be excluded completely. A research activity has started some years ago in the framework of collaboration between the ENEA (Italy) and the SRI (USA), aimed to the identification of traces of nuclear reactions in condensed matter. Preliminary results 1 by Neutron Activation Analysis (NAA) have given indication of Ag isotopic shift occurring in Pd thin films after electrolysis. A first screening by Secondary Ion Mass Spectrometry (SIMS) of the isotopic composition of Nickel thin films undergone to similar experiments has also pointed out an isotopic ratio different from the natural one on the 63/65 masses imputable to copper. 2 In this work, further reproduction of the previous experiments and a more accurate analysis of the experimental data have been performed. Cross-linked analysis has also been involved, in order to identify artifacts that could affect the isotopic shift estimate.

2. Experimental The typical experiment, already described in Ref. 2, consisted in three steps: • Deposition of two identical Reference and Active nickel films during the same deposition run; • Hydrogen loading of the Active film by electrolysis; • SIMS analysis of both Reference and an Active sample isotopic composition, to search deviations from the natural abundances.

266

Steps (1) and (2) have been carried out in a class 1000 clean room laboratory, by using clean room grade gloves and papers in order to reduce source of contaminants. To the same aim, a reduced number of high-purity materials have been used both for sample production and electrolysis cell assembling. 2.1. Metallic

Film

Deposition

The films (with 45 nm thickness) have been deposited by ion beam sputtering of a Ni target (MRC, 99.98% purity) on polyethylene (kartell) 12 mm diameter - 1 mm thick disks. Before deposition, the substrates have been chemically cleaned as reported in Ref. 2, and ion beam etched to improve film/substrate adhesion and to assure good film surface status after electrolysis.Up to six identical Reference and an Active nickel films have been deposited during the same run, loaded on a rotating sample holder. 2.2. Hydrogen

Loading

The hydrogen loading of the Active film has been carried out by electrolysis, in Light water (18 MW) LiS04 solution (1M). The cell was realized in polyethylene (Kartell), with high purity (99.98%) Pt electrodes (see photo in Ref. 2). Typical values of the current and voltage used during the experiments ranged between 5190 mA and 2-7 V, respectively. Loading times went from a minimum of 3 h to a maximum of 40 h. 2.3. SIMS

Analysis

Secondary Ion Mass Spectrometry measurements have been carried out with a Leybold SSM-Mass Spectrometer Module, operating at the ENEA research centre in Frascati (Rome, Italy). The Mass Spectrometer is equipped with a source Leybold IQE 12/38 ion source and a Balzers Quadrupole Mass Analyser working in the mass range 0-511 a.m.u. The primary beam was fed by Ar + ions at 5keV. The beam spot had a diameter of about 2 mm, small enough to allow scanning of the sample surface. Typical sensitivity and resolution were 0.5 a.m.u. (m/ Ni 58 Li 7 , mass 67 =4> Ni 60 Li 7 , mass 82 => Ni 58 Li 7 OH, mass 84 =>• Ni 60 Li 7 OH). In Table 3 are reported the intensity ratios between the SIMS peaks associated with the above compounds. The obtained values match the natural isotopic ratios in the case of the Ni 58 and Ni 60 isotopes, but nothing can be said in the case of Li 7 , Li6 isotopes, due to the poor accuracy of the data, affected by the Ni 64 contribution to the 64 peak. In conclusion, the contribution to the 65 mass peak from Ni 58 Li compound seems to be the only reasonable explanations of the reported results, out of the copper isotopic shift hypothesis. This supposition could also be consistent with the SUPER-SIMS results, which indicated a value for the isotopic composition of copper similar to the natural one for both the active and reference films analyzed. Some uncertainty still affect our results, concerning the fact that Li contamination from the electrolyte is expected in all electrolyzed samples while in some of them the 65 extra signal has not been revealed. As concerning the SUPER-SIMS measurements, the information is limited to a restricted area of the film surface, because only one point of the surface of each sample has been analyzed, which could be not representative of the whole sample surface, since a gradient effect in the isotopic composition has been demonstrated by the conventional SIMS surface scanning analysis. Further experiments and tests could be useful in the future, to completely understand the present data. In particular, surface scanning by ultra-high resolution SIMS apparatus (m/ 3000, enough to resolve mass interferences), Table 3. Intensity ratios between the SIMS peaks associated with the NiLi and NiLiOH compounds Isotopes ratio

SIMS peaks ratio

Natural isotopic ratio

Ni58Li7/Ni60Li7 Ni 5 8 Li 7 OH/Ni 6 0 Li 7 OH Ni58/Ni60

2.0 ± 0.5 2.5 ± 0.5 2.71 ± 0 . 0 1

2.60 2.60 2.60

271

cross-matched analysis by other methods (e.g. Nuclear Activation Analysis), similar experiments with changed electrolyte (e.g. N a O H instead of LiS04).

5.

Conclusions

Based on preliminary results, showing evidences of isotopic shift on the Cu masses (65 too high) in Ni hydrogenated films, a new set of experiments has been reproduced and further analysis have been performed in order to exclude t h a t the revealed shift was traceable to an artifact. These included SIMS scanning of the sample surface, depth profile analysis by SIMS, mass spectrometric analysis of the electrolyte, SUPER-SIMS analysis of one couple of reference and active films. On the basis of the new results, a more complex scenario has been evidenced, suggesting t h a t the former attribution of the C u 6 3 / C u 6 5 isotopic shift could be not correct. T h e work wants to stress t h a t the identification of elemental transmutations in metal hydrides is an extremely complex topic, which necessitate of severe scientific accuracy, cross-matched analysis, multidisciplinary expertise and the access to top performance experimental facilities. All these requirements can be fulfilled only in the framework of top-level scientific collaboration worldwide.

Acknowledgments T h e authors t h a n k Dr. K. Grabowski and Dr. M. Melich of Naval Research Laboratory (Washington, DC, USA) for the important help received on this matter. T h e contribution of Dott. Luigi Nardi of E N E A research center Casaccia (Rome, Italy) in performing the gas cromatography analysis is sincerely acknowledged.

References 1. V. Violante, M. L. Apicella, L. Capobianco, F. Sarto, A. Rosada, E. Santoro, M. McKubre, F. Tanzella, and C. Sibilia - Search for nuclear ashes in electrochemical experiments. Proc. of 10th International Conference on Cold Fusion (ICCF-10), Cambridge, MA, August 24-29 (2003), World Scientific Inc., Singapore. 2. SUPER-SIMS analysis has been performed by the facility located at ETH, by Dr. M. Doebely. 3. V.Violante, P.TYipodi, D. Di Gioacchino, R. Borelli, L.Bettinali, E.Santoro, A. Rosada, F.Sarto, A.Pizzuto, M.McKubre, F.Tanzella, X-ray emission during electrolysis of light water on palladium and nickel thin films. Proc. of 9th International Conference on Cold Fusion, (ICCF9), Beijing, May 19-24 (2002). 4. SIMS technical report by RIBER Instrumentation Ultra-vide, France. 5. Integrated Spectral Data Base System for Organic Compounds by National Institute of Advanced Industrial Science & Technology, SDBSWeb: http://www.aist.go.jp/ RIODB/SDBS/. 6. Organic Compound Database by Harold M. Bell at Virginia Tech., http://www.colby. edu/ chemistry/cmp/cmp.html.

IN SITU ACCELERATOR ANALYSES OF PALLADIUM COMPLEX UNDER DEUTERIUM PERMEATION

A. K I T A M U R A , R. NISHIO, H. IWAI, R. SATOH, A. TANIIKE A N D Y. F U R U Y A M A Department of Environmental Energy Science, Graduate School of Science and Technology, Kobe University, 5-1-1 Fukaeminami-machi, Higashinada-ku, Kobe 6580022, Japan E-mail: kitamura@maritime. kobe-u. ac.jp

Preliminary results of experiments on D2 gas permeation using a system (vacuum/CaO/Sr/PdD a ; /D2) have shown some evidence of nuclear transmutation from Sr to Mo. The system is a little simpler than that used by Imamura et al., and has a reversed gas flow direction. The diagnostic method used to identify the elements was conventional X-ray photoelectron spectroscopy, giving the areal densities of 4.2 X 10 1 4 c m " 2 (Sr) and 3.3 X 10 1 4 c m " 2 (Mo). Extended analytical methods are now being prepared, including in situ and simultaneous particle induced X-ray emission, Rutherford backscattering spectroscopy, nuclear reaction analysis, and elastic recoil detection analyse for areal densities of transmutation elements and deuterium distribution.

1. Introduction It has been claimed 1 ' 2 that forced permeation of deuterium through P d / ( C a O + P d ) / P d samples doped with some element X induced nuclear transmutations from X to X', where (X, X') being ( 133 Cs, 1 4 1 Pr), (88Sr, 96 Mo), ( 138 Ba, 150 Sm), and ( 137 Ba, 149 Sm). The main diagnostic methods in these studies were X-ray photoelectron spectroscopy (XPS), time-of-flight secondary-ion mass spectroscopy (TOF-SIMS), and X-ray fluorescence (XRF). To confirm and investigate the phenomena, it is essential that the same results be obtained in different laboratories with different analytical methods. We have constructed an experimental system, with which accelerator analyses of the samples including particle induced X-ray emission (PIXE), elastic recoil detection analysis (ERDA), nuclear reaction analysis (NRA), and Rutherford backscattering spectroscopy (RBS) can be made in situ and simultaneously with gas permeation through the samples. In the present work, we use a sample similar to, but somewhat different from those used in Refs. 1 and 2: vacuum/CaO/Sr/PdD a ; /D2. Here we report preliminary experimental results on the transmutation diagnosed by conventional XPS method. Results from the in situ analyses will be published later, elsewhere. 272

273

I 0

I 2

I

I

I 4

I 6

l

I 8

l 10

Time [s] Figure 1. (a) Schematic of deuterium permeation in situ accelerator analyses system, (b) the CaO/Sr/PdDj; sample structure, and (c) electrochemical method used for Sr deposition onto the Pd sample.

2. Permeation in situ Analysis System and Sample Preparation The experimental setup is shown in Fig. 1. The multi-layered sample is placed at the center of the vacuum chamber. The sample surface can be diagnosed in situ with probe beam ions to emit characteristic X-rays, which are analyzed either with a CdTe detector or a Si-PIN-type X-ray detector positioned at 150° relative to the probe beam direction. Additional solid-state charged-particle detectors are provided for RBS, ERDA, and/or NRA characterization of the sample. The multi-layered Pd samples were prepared as follows. The Pd sheets of 33 x 33 x 0.1mm 3 were annealed for 3h at 570 K after 1-second immersion in aqua

274

regia/D20. Sr atoms were then deposited on one side of the Pd surface using a method similar to electroplating: as shown in Fig. 1(c), the Pd sheet was carefully placed on the surface of the 10 mM Sr(N03)2/D20 solution, so that only one side of the sheet was in contact with the solution. A bias voltage of 1V was applied between the Pd cathode and a Pt anode wire immersed in the solution. The ion flow onto the Pd cathode was appreciable only at the beginning of the electroplating process, as can be seen in the graph, implying a saturation of the surface with contamination layer containing Sr. Neither further increase in the processing time nor multiple immersions and biasing resulted in any increase in the areal density of Sr deposited. Next, a CaO layer was deposited on the Sr/Pd surface by RF sputtering for 5-20 min. The thickness of the CaO layer was deduced from variation of the XPS spectral intensities. As shown in Fig. 2(a), the peak intensities of Pd-3d and Ca-2p photoelectrons vary with surface etching time. The CaO layer thickness x is calculated from the intensity ratio of these peaks, Ica^p/ypd-sd: using the following equation: exp

, AcaO-Pd J \

1 — exp

*" V

_ AcaO-Ca J J

" P d #S»> Ssxtelt* ( r f e r«nt[f- l l f t i

>

Q u n o o D %— 30D 6

J o n C u r r e n t IF

r u m - f i t IF 09A1

I o n C u r n - n l [A,

4U0O 3000 ZOOO-

95 0

IDS II

200 B

203 0

308 S

303 0

Figure 3. Plots of QMS analysis. First row—original deuterium gas; second row—gas sample permeating through P d film; third row—mass 3 peak in linear scale for gas sample permeating through Pd film; fourth row—standard helium 3 gas.

282

gen molecules (H 2 ), which was released from the stainless steel parts of Swagelok connection due to the heating (330°C). However, one might still wonder if there was any helium-3 or tritium involved in peak of the mass 3. In the third row and the fourth row of Fig. 3, standard helium-3 sample was used to calibrate the peak position of mass 3. The logarithmic scale in ordinate was switched to linear scale in order to clearly show the peak position. The third row shows the mass 3 peak from the gas sample permeating from the palladium film, and the fourth row shows the helium-3 peak from the standard helium 3 sample [m(3He) = 3.016], which is on the left-hand side of the mass 3 peak in the third row. It is clear that the major part of mass 3 peak in the third row is from the DH + [m(DH) = 3.021] due to the Longevine effect. The mass 1 peak supports this assumption of residual hydrogen gas during the heating. Nevertheless, we might suspect if any helium-3 was covered by the strong HD peak. In Fig. 4, a careful analysis was done for the strong peak in mass 3. The width of the slot in front of the Faraday collector in QMS was narrowing down gradually in order to improve the resolution further at the cost of reducing sensitivity.

E-13-i

300

I, i , i • i ,

301

302

,

303

304

i

305

Figure 4. Mass 3 peak was re-analyzed in terms of narrowing slot in Faraday collector. A turning point appeared near the 3.016 might imply a trace of helium-3 covered by strong HD peak.

283 Acknowledgments This work is supported by the Natural Science Foundation of China (no. 10475045), Ministry of Science and Technology (Division of Fundamental Research), and Tsinghua University (985-11, Basic Research Funds).

References 1. A.H. Verbruggen et al, Phys. Rev. Lett. 52, 1625 (1984). 2. P.H. Dawson, J. Vac. Sci. Technol. 11(6), 1151 (1974). 3. B. Liu, X.Z. Li et al, in: A. Takahashi, Y. Iwamura, and K. Ota (eds), Proc. ICCF-12, Yokohama, Japan (Nov. 27-Dec. 2, 2005). 4. P. Langevin, Ann. Chem. Phys. 5, 245 (1905). 5. X.Z. Li, G. L. Schmidt and J. Tian, The Proceedings of the 5th Asti Workshop on Anomalies in Hydrogen/Deuterium Loaded Metals, Asti, Italy (19-21 March 2004). 6. Q.M. Wei, X.Z. Li et al, in: J.-P. Biberian (ed.), Proc. Iccf-11, Marseilles, France (31 Oct.-5 Nov. 2006, 2004), p. 351.

ICP MS ANALYSIS OF ELECTRODES A N D ELECTROLYTES A F T E R H N 0 3 / H 2 0 ELECTROLYSIS

S. T A N I G U C H I , S. S H I M A D U , H. Y A M A D A A N D S. N A R I T A Department

of Electrical

and Electronic Engineering, Iwate Morioka 020-8551, Japan E-mail: [email protected]

University,

Ueda If-3-5,

T . O D A S H I M A A N D N. T E S H I M A Department

of Chemical

Engineering, Ichinoseki National Takanashi, Ichinoseki 021-8511,

College of Technology, Japan

Hagiso,

T. O H M O R I Advanced

Technology

Inc., Hokkaido Institute Sapporo 006-8585,

Technology, Japan

Maeda

7-15,

Teineku,

We carried out light water electrolysis with Pd cathode and Pt anode. The composition of both electrodes and the electrolytes were analyzed by Inductively Coupled Plasma-Mass Spectrometry to search for the evidence of the nuclear transmutation. In the light water electrolysis experiment, various elements have been observed on the metallic electrodes and in the solution after the electrolysis. In particular, amount of P b increased remarkably after the electrolysis, and this result gave good reproducibility. There was no difference between the isotopic ratio of P b detected and natural one

1. Introduction In light water electrolysis experiments, elements production has been reported. 1 In most of them, only the surface compositions of the electrodes were analyzed. In addition to analysis of the electrodes, it is desirable to investigate electrolytes since elements on/in the electrodes can be dissolved in it. In this study, both solutions of electrodes and electrolyte were analyzed by Inductively Coupled Plasma-Mass Spectrometry (ICP-MS)(SII : SPQ9000). The sample solution introduced into the ICP MS should be acid in general. Then, we utilized HNO3/H2O as electrolytic solution instead of Na2S04/H 2 0 or K2SO4/H2O, that we previously used in our experiment so that the electrolytes can be directly introduced into the device. 2. Experimental We employed a PTEF test cell in this study. The cell is shown in Fig. 1. The cell was 73 mm in diameter, 175 mm of height, and cylindrical shape with volume capacity of 500 ml. The Pd foil (99.95% pure) for cathode was 0.1 x 5x10 mm 3 in 284

285

size and the Pt foil (99.98% pure) for anode was 0.1 x 5 x 10 mm 3 in size. The gap was about 3 cm. A Pd lead wire (4>1 mm) and a Pt lead wire (<j>l mm) were used for connecting cathode and anode to a power supply, respectively. They were coated with Teflon heat-shrinkable tubes. Before the electrolysis, the electrodes were washed with acetone and aqua-regia to remove the impurity. The electrolytes used were ultrapure nitric acid (Ultrapure reagent, Kanto kagaku, Tokyo, Japan). The volume of electrolyte solution was 500 ml. J DC 2 or 1 A

Pt (i|>1 mm) Pd (1 mm)

, Cathode

Pd

^

Anode

3 cm

(0.1 x5x10mm)

< Pt to 1 x5x10mm)

(a)

(b) Figure 1.

P T F E cell.

In the electrolysis, 0.1 M HNO3/H2O was used and DC 1 or 2 A was applied for 14 days. 2 The cell was replenished with ultra pure water of 100-200 ml every day. The electrodes (we call it "After sample") were cut off from the lead wires, after the electrolysis. We prepared reference sample, which was just soaked into the electrolyte for 14days (we call it "Before sample") without supplying the current. We used this cell as an open-cell. The pressure inside cell was kept to be slightly higher than atmospheric pressure during the electrolysis.3 The cell was set in an outer container. Moreover, whole the container was set in a box to avoid contamination. The temperature inside of box was kept constant at 15°C. The elemental analysis of the electrodes and electrolyte was examined by ICP-MS. It can detect the most of elements with high sensitivity (~ppb) and measure the density in the sample for specified elements. It can also evaluate the isotopic abundance. 3. Results and Discussion 3.1. Change in Weight and Thickness

of

Electrodes

In pre-processing of ICP-MS analysis, the Pd and Pt electrodes were immersed in 1 ml of ultra pure nitric acid for 10 s to dissolve most of all the elements on the surface of samples in the nitric acid. Then pure water was added to the nitric acid solution to be totally 50 ml of more thin acid solution for the processing ICP-MS. In the processing, a semi-quantitative and quantitative analysis was done by ICP-MS in this research.

286 Table 1.

Change in weight and thickness of electrode

Current (A)

Pt (before)

P t (after)

Pd (before)

Pd (after)

2 Amount dissolved (mg) 0.04 Depth (nm) 19.0

0.01 4.7

0.56 5.0 X 10 2

0.49 4.0 X 10 2

1 Amount dissolved (mg) Depth (nm)

0.02 9.4

0.20 2.0 x 10 2

0.02 16.4

0.02 9.4

To estimate the depth of samples dissolved in the nitric acid, we compared the weight of samples before the pre-processing with that after the pre-processing. The depth was calculated using the density of the electrodes, 21.37g/cm 3 for Pt and 12.16g/cm 3 for Pd. Table 1 shows the amount dissolved and the depth of Pt and Pd electrodes in HNO3. After treatment by the nitric acid, the dissolved amount for both "Before samples" of Pt and Pd is large than that for "After samples" under the test condition of current 2 A. In case of current 2 A for Pd sample, the dissolved amount 0.56 mg of "Before sample" and that 0.49 mg of "After sample" correspond to dissolved depth 5.0 x 102 and 4.0 x 102 nm, respectively. This indicates that amount of impurity from "After sample" of Pd should be less than that of "Before sample" of Pd. Under the same test condition of 2 A for Pt, similar result can be deduced from comparing weight of "Before sample" with that of "After sample". 3.2. Elements Newly Detected Electrolysis

and Increased

after

HNOz/H^O

All the elements with mass number from 6(Li) to 238(U) can be detected in a run of the ICP-MS with high sensitivity (ppb). In our analysis, the signal stands out when the corresponding element exists with the density above 0.1 ppb. Element Pb was newly detected by the ICP-MS only after electrolysis as shown in Table 2. In particular, marked count of Pb was observed in electrolyte after electrolysis for 1 A. To the contrary, no count was observed on both electrodes and in electrolyte for the "Before samples", as seen in this table. Furthermore, we analyzed the amount of Pb in bulk Pd piece of 29.50 mg and Pt piece of 52.41 mg after each whole piece volume was dissolved in the aqua-regia, and have found no count of Pb in these pieces by Table 2.

Density of P b in the thin nitric acid solutions and electrolytes

Current (A)

Pt (before) (ppb)

Pt (after) (ppb)

Pd (before) (ppb)

Pd (after) (ppb)

Electrolyte (before) (ppb)

Electrolyte (after) (ppb)

Pb 2 1

— —

— 2.7842

— —

9.1406 6.7815

— —

6.401 14.1592

287 8.0

• 2A

6.0

5 4.0 2.0

0.0 Pt (Anode)

Figure 2.

Electrolyte

Amount of P b on the electrodes and in electrolyte.

ICP-MS. It should be noticed that the change in weight of "Before sample" was larger than that of "After sample" for both Pt and Pd electrode, as mentioned above. From these results, it is unlikely that those Pb was impurity originating from bulk Pd and Pt electrodes. Since the volume of electrolyte is 10 times larger than that of the thin acid solution, the amount of Pb in the electrolyte is larger than these on electrodes. On the other hand, the density of Pb in air environment is generally thought to be 0.6 ng/m 3 . 4 Taking account of this low value, the Pb detected in this experiment is not considered to be impurities from the air environment. The deduced amount of Pb from the density values in Table 2, on both electrodes and in the electrolyte, is given in Fig. 2.

3.3. Isotopic

Distribution

of Pb

Table 3 shows counts of Pb on electrodes and in electrolyte after the electrolysis, using ICP-MS. The isotopic distribution deduced from the values in the table is presented in Fig. 3. The isotopic distribution of Pb obtained is close to the natural isotopic one.

Table 3. Count of P b in the thin nitric acid solutions and electrolytes

204

Pb Pb 207 Pb 208 Pb

206

(cps) (cps) (cps) (cps)

Pt (after)

Pd (after)

Electrolyte (after)

526.2 9069.5 8022.0 19429.4

1250.6 23567.1 20306.7 50040.5

3282.3 59884.1 50478.0 128258.3

288

Pt (Anode)

Figure 3.

4.

Pd (Cathode)

Electrolyte

Isotope distribution of P b in the thin nitric acid solutions and electrolytes.

Conclusion

We have analyzed the P d and P t electrodes and H N O 3 / H 2 O electrolyte after the light water electrolysis. (1) No element P b was observed on b o t h electrodes and in electrolyte before the electrolysis. (2) Considerable amount of P b was detected on b o t h electrodes and in electrolyte only after the light water electrolysis. (3) T h e isotopic distribution of P b is close to the n a t u r a l isotopic one. (4) Element P b detected is possible candidate of product resulting from low energy nuclear reaction.

References 1. J. Dash, R. Kopecek, and S. Miguet, The 32nd intersociety energy conversion engineering conference, vol. 2, pp. 1350-1355 (1997). 2. H. Yamada, S. Narita, Y. Fujii, T. Sato, S. Sasaki, and T. Omori, Proc. 9th International Conference on Cold Fusion, pp. 420-423 (2003). 3. T. Sato, S. Sasaki, T. Kubozono, S. Narita, H. Yamada, and T. Ohmori, Proc. J^th Meeting of Japan CF Research Society (October 17-18, 2002), pp. 9-12. 4. The periodic table of the elements, http://home.hiroshima-u.ac.jp/er/ Rmin_GL.html#anchor646130

THE ITALY-JAPAN PROJECT FUNDAMENTAL RESEARCH ON COLD T R A N S M U T A T I O N P R O C E S S FOR T R E A T M E N T OF NUCLEAR WASTES

AKITO TAKAHASHI Osaka University,

2-2 Yamadaoka Suita, Osaka 565-0871, E-mail: [email protected]

Japan

FRANCESCO CELANI INFN,

Via Enrico

Fermi,

40-00044

Frascati

(Rome),

Italy

YASUHIRO IWAMURA Mitsubishi

Heavy Industries

Ltd.,

16-5, Konan Japan

2-chome,

Minato-ku

Tokyo

108-8215,

The IJ Project proposes, as the first phase of research, that confirmation of the cold transmutation using radioactive isotopes such as 1 3 7 C s , 9 0 Sr, and 1 3 6 Cs to non-radioactive elements will be implemented based on the Mitsubishi Heavy Industries, Ltd. (MHI) method. A theoretical background has been given by the TSC-induced nuclear reactions (Proc. ICCF 10). Charge-neutral pseudo-particle of 4d/TSC can become as small as 10 fm radius in its minimum state of squeezing motion, and will make 4D-capture reaction with host metal (or added metal) nuclei in the surface region of permeation {Proc. ICCF 9, 10) samples. Major reaction will be: M(A, Z) + 4 d / T S C - • M(A + 8, Z + 4) + Q. Theoretical modeling of the process is briefly explained and resulting reaction products, their decays and final stable isotopes are predicted for 1 3 7 Cs, 9 0 Sr, and 135 Cs transmutation.

1. Introduction Recent studies on condensed matter nuclear effects in/on near surface regions of metal deuterides and hydrides have provided some confident experimental results about occurrence of cold transmutations in condensed matter containing deuterium and hydrogen. 1_3 Especially the latest works by Iwamura et al.4'5 are novel enough to be considered important new findings in condensed matter nuclear effects. Iwamura et al. have repeatedly shown that there occurs selective transmutation from 133 Cs to 1 4 1 Pr (or 88 Sr to 96 Mo) in the experimental system of D-gas permeation through Pd-complex samples. Pd-complex samples are made with multilayered P d / C a O / P d plates in nm size processing. The IJ-Project aims at confirming the selective transmutation process by using special samples containing radioactive Cs and Sr. This is a pure basic science project. 289

290

2. Selective Transmutation This new type of transmutation is the process of adding 4D or 8 Be to the host element M(A, Z) and to transmute to M'(A+8, Z+A). Therefore, some kind of coherent multi-body process in condensed matter should exist as the underlying physics mechanism. One theoretical interpretation has been proposed by Takahashi. 6 A theoretical background has been given by the TSC-induced nuclear reactions. 3 Charge-neutral pseudo-particle of 4d/TSC can become as small as 10 fm radius in its minimum state of squeezing motion and will make 4D-capture reaction with host metal (or added metal) nuclei in the surface region of permeation 1,2 samples. The major reaction will be: M(A, Z) + 4d/TSC - • M{A + 8, Z + 4) + Q.

(1)

7

Iwamura et al. has also reported that 6D added transmutation. Takahashi 6 has proposed a model for 6D/OSC process to interpret it. If we do experimental tests using radioactive samples of, e.g., 137 Cs, 135 Cs, and 90 Sr to confirm a significant decrease of their radioactivity, the transmutation effect will be clearly confirmed in the view of nuclear science. Then we may consider the possibility of applying the process to the remediation for long-lived radioactive wastes from nuclear plants, although that would require a drastic scale up of transmutation rates compared with the original claim by Iwamura et al. 3. Model of TSC-induced Transmutation According to the Takahashi model of TSC-induced reaction, 4D/TSC at its minimum-size state of squeezing motion may behave as a very small (about 10 fm in diameter) pseudo-particle of neutralized electric charge. A model of formation mechanism on surface of Iwamura sample is shown in Fig. 1. Surface elements analysis by TOF-SIMS by Iwamura 5 and Takahashi 7 revealed that supposed transmutation took place within 10 nm depth zone from surface of Pd-complex sample plate. Figure 1 models some sites like corner holes to provide site for TSC formation. Then TSC squeezing motion produce TSC-minimum-size state of about 10 fm diameter to approach and make strong force exchange with host metal nucleus as shown in Fig. 2. The capture reaction rate for the process of Fig. 2 can be approximately estimated by STTBA. 6 ' 7 For the 133 Cs + 4d/TSC to 1 4 1 P r + Q process, 4.6 x 10 14 Pr-atoms/week/cm 2 is estimated 6 and this value is close to Iwamura results. 4 4. Prediction for Radioactive Samples The reaction scenarios by TSC-induced transmutation predict the following reactions and products for 137 Cs, 135 Cs, and 90 Sr being considered for the IJ-Project. 133

Cs + 4d/TSC -^ 1 4 1 Pr(Ex = 50.49 MeV) -> FPs 141

Pr(stable) + gammas,

or (2)

291

Image of surface Dimer •

/

/o

W

W

w

o _o^o

o• o •

• °„ •o o O

A

° o°

W

•

« U

o! W • -

Adatom

>

*^

o*>«-

Corner-hole with dangling-bonds

°2W TSC is born here?

o

. Pd

CaO

Figure 1.

137

^BF Cs

O Deuteron

Model of surface of Iwamura type sample.

Cs- 4d/TSC -^ 1 4 5 Pr(Ex = 45.63MeV) - • Fission - Products (in 10fs) 145

Pr(5.98 h)

145

or

Nd(stable) + gammas (in few fs).

(3)

During the beta-decay of 1 4 5 Pr with 5.98 h half-life, there should be a small fraction (1%) of gamma-rays at £ 7 = 675.8 and 748.28 keV, which we can detect with HpGe detector to identify the occurrence of reaction (3). 135

Cs + 4d/TSC ^ 1 4 3 Pr(Ex = 48.03 MeV) - • Fission-Products (in f 0 fs) 143

90

or

Pr(f 3.57days) 143 Nd + gamma (in few fs),

(4)

Sr + 4d/TSC ^ 9 S Mo(Ex = 54.71 MeV) -> Fission-Products (in 10 fs) or 98

Mo(stable) + gammas (in few fs).

(5)

For all cases, fission channels may be opened due to very high-excited energies of intermediate compound nuclei. However, we predict gamma transitions will be more dominant than fission, due to shorter transition times (few fs) than about 10 fs life for fission break up by collective deformation of excited nuclei (dumbbell oscillation). Gamma-transition from highly excited states may emit very high-energy gamma quanta in about 50 MeV range. To detect and identify these very high-energy gamma-rays is difficult and money consuming effort is needed, because the process for detection is mostly by Compton scattering and we do not have definite method

292

M-nucleus

Figure 2. Strong interaction (PEF) between TSC-minimum-size and host-metal M-nucleus. The admixture of 4d/TSC forms 8 Be* compound state for short time.

for unfolding broadened pulse height spectra of observation with usual detectors (Nal, Ge, etc.). 5. C o n c l u s i o n s (1) T S C as small neutral pseudo-particle induces nuclear reaction with host metal-nucleus. (2) Cold t r a n s m u t a t i o n by high-energy 4 H e and 8 B e particles by self-fusion of 4 d / T S C is also predicted. (3) Cold t r a n s m u t a t i o n by T S C + Host-nucleus by (1) will be almost nonradioactive. (4) Confirmation by the IJ Project is expected. (5) If confirmed, a scale-up study is expected. References 1. Proc. ICCF9, Tsinhua University Press (see also; http://www.lenr-canr-org/). 2. Proc. ICCF10, Boston (2003) to be published (see also the above site). 3. Proc. ICCF11, Marseilles (2004) to be published (see also the above site and http://www.iscmns.org/). 4. Y. Iwamura et al, Jpn. J. Appl. Phys. 4 1 , 4642 (2002). 5. Y. Iwamura et al., Proc. ICCF10, Boston (2003). 6. A. Takahashi, TSC-induced nuclear reactions and cold transmutations, Proc. Siena Workshop, http://www.iscmns.org/ (2005). 7. A. Takahashi, Recent Res. Dev. Phys. 6, 1-28 (2005).

R E P R O D U C I B L E N U C L E A R EMISSIONS FROM Pd/PdOiDa: H E T E R O S T R U C T U R E D U R I N G CONTROLLED E X O T H E R M I C DEUTERIUM DESORPTION

A . G . L I P S O N A N D G.H. M I L E Y University

of Illinois at Urbana- Champaign, Department of Nuclear, Radiological Engineering, Urbana, IL 61801, USA E-mail: [email protected]

Plasma

and

A.S. R O U S S E T S K I P.N. Lebedev Physics

Institute,

Russian

Academy

of Sciences,

Moscow

119285,

Russia

199991,

Russia

A . G . L I P S O N , B . F . L Y A K H O V A N D E.I. S A U N I N Institute

of Physical

Chemistry,

Russian

Academy

of Sciences,

Moscow

Weak nuclear emissions accompanied deuterium loading/deloading into Ti and Pd matrix have been studied for more than a dozen years. PdDa; sample subjected to electrochemical/gas loading or deuterium desorption/deloading generate weak random fluxes of DD-reaction products (neutrons and protons) and energetic alpha particles. However, reproducibility of these emissions was low depending on material quality and experimental conditions. Here we present new reproducible results on DD-reaction products, energetic alpha particles and soft X-ray emissions detected in controlled conditions of exothermic deuterium desorption from the surface of Pd/PdO:Da; heterostructure.

1. Introduction Weak nuclear emissions accompanied deuterium loading/deloading into Ti and Pd matrix have been studied for more than a dozen years. 1 ' 2 It was found that in some cases neutrons and charged particles (protons and tritons) are observed in Pd cathodes during electrolysis, glow discharge bombardment and deuterium desorption from these samples. The rate of those emissions considering as a signature of low-energy DD-reaction is very low and still unpredictable. This indicates low reproducibility of low-energy DD-reaction in deuterium-loaded metals and makes doubtful existence of entire low-energy nuclear processes in non-equilibrium solids. Moreover, the existence of nuclear processes of any type in D-loaded Pd requires observation of X-rays accompanying charged particles braking in solids. So far, there were no unambiguous reports concerning X-ray generation from PdDa; during and after electrochemical loading with deuterium. Meanwhile, earlier we just have reported observation of 2.45 MeV neutrons and high-energy alpha particles during exothermic deuterium desorption from specially 293

294

prepared Pd/PdOiDz heterostructure. 3 ' 4 It was also shown that Pd/PdO samples demonstrate highest screening potential and highest deuterium diffusivity (compared to other metals including pure Pd) in experiments on 2.5-10 keV deuteron bombardment with accelerator. 5 ' 6 These facts allow to assume that Pd/PdO:Da; heterostructure samples could serve as a good candidate to achieve reproducible LENR effects in exothermic deuterium desorption process, including both nuclear and X-ray emissions. Thus, to verify our assumption concerning unique nuclear properties of Pd/PdO:Da; system during D-desorption the objectives of this research were directed to: • Obtain reproducible nuclear emissions in controlled conditions of exothermic D-desorption from PdO/Pd/PdOiDrr heterostructure. • DD-reaction yield (3.0 MeV protons). • Energetic alphas. • Soft X-rays. • Control of sample temperature and D-desorption rate on-line. • To figure out how these emissions could be linked via D-desorption. In the present paper, we show new reproducible results on DD-reaction products, energetic alpha particles and soft X-ray emissions detected in controlled conditions of exothermic deuterium desorption from the surface of Pd/PdChDa, heterostructure. 2. E x p e r i m e n t a l The samples of Pd/PdO were synthesized by thermal growing of thin oxide layer (PdO y ) of 20 nm thick on top of 110 ^m thick annealed cold worked Pd foils (area 2.3 x 1.1cm2) using an oxygen-propane torch. The electrochemical loading of Pd/PdO cathodes by x = D/Pd = 0.7 has been carried out with low current density (j ~ 20mA/cm ) electrolysis in lM-LiOD/D20 solution using a special cell with divided cathode and anodic spaces. Immediately after achieving an x = 0.7 loading ratio, the electrolysis was interrupted. The Pd/PdOiDa, sample with attached CR-39 or thermal luminescent (TLD) detectors is placed under mechanical loading (m = 150 g) for one hour at T = 20°C. During this time the Pd/PdOiDz sample showed signs of heating up to 7.0°C caused by exothermic deuterium desorption. Loading ratio x = D/Pd has been measured using both thermal desorption and anodic polarization techniques. 2 In order to determine x = D/Pd value, the sample was underwent by vacuum heating or anodic polarization after each cathode loading time interval t. About 90% of initial deuterium content was found to be desorbed through Pd-PdO interface during t = 1.0 h. In control experiments a similar Pd/PdO sample electrochemically loaded with hydrogen in 1-M NaOH/H 2 0 electrolyte and exposed to CR-39 detectors has been employed. In blank/background experiments, unloaded Pd/PdO heterostructure samples were used with CR-39.Both open and filtered CR-39 track detectors have been applied in our experiments in order to estimate type and energy distributions of emitted

295

particles. The photo-insensitive X8 LiF TLD (Landauer) units used for soft X-ray detection were filtered by 1-4 layers of 15 /im polypropylene. 3. Experimental Results Kinetics of integral deuterium desorption from Pd/PdO:Da; and its rate for first 70 min after exposure are shown in Fig. la and b, respectively. As seen, the desorption rate demonstrate maximum near t — 10-15 min elapsed after the loading interruption. It was also found that about 90% of all deuterium absorbed by P d / P d O sample leaves heterostructure during 60 min of its exposure at room temperature. During D-desorption the ambient temperature and temperature of the sample were measured simultaneously using to independent thermocouples. It was found that from the start of exposure in air atmosphere (immediately after interruption of loading and drying the sample) the temperature of Pd/PdO:Dir sample jumps five degrees above the ambient one (Fig. 2). The temperature of the sample has tend to increase two degrees more during following 20 min and then exponentially decreases with decrease in loading ratio x = D/Pd and (Fig. la) and desorption rate (Fig. lb). Notice that shape of the Pd/PdO:D:r T(t) (Fig. 2) curve is roughly repeat the shape of desorption rate curve (Fig. lb). The coincidence of T(i) and desorption rate curves give rise to conclusion that observed heating of the sample is referred to exothermic deuterium desorption from the surface of Pd/PdO:Da; heterostructure in air (oxygen) atmosphere. In this condition the PdO surface may catalyze exothermic D + D —> D2 +Q moleculization reaction at room temperature. Pd/PdO:Dj; runs with CR-39 detectors showed a highly reproducible yield of 3 MeV protons from DD-reaction accompanied by energetic alpha emission in the range of 11-16 MeV. These emissions are not detected in the blank experiments with unloaded Pd/PdO heterostructure. Integral charged particle spectra obtained with open CR-39 detectors (without filter) during 12 runs with duration ~ 1 h 0,025

& 0,020 •

x=D/Pd measurement Exponential fit

1 '

3 ' "

0 3

• I •/ I 0,015 . \ 1

Ii

\

§ 0,010

i \ •

D.

° 0,005 o

I—J 1 0,000

0,0-

10

20

30

40

50

60

70

80

• ^

4.1.

i

10

20

—

>

—

i

—

i

30

—

i

40

—

i

—

i

50

Elapsed time (min)

Elapsed time (min)

(a)

(b)

—

i

—

60

70

Fig. 1. Integral deuterium desorption (a) and desorption rate (b) from 110 (an P d / P d O i D x heterostructure electrochemically loaded with deuterium versus elapsed time at T = 18°C. Notice that ~ 90% of absorbed deuterium escapes the sample during 1 h of its exposure.

296

OA m

y •s

0*3 • c.O "

9

2?-

3

•

s

• Sample temperature —•—Room temperature

/i

on. |600V are observed with a discharge voltage only about half of that value. To further investigate this phenomenon, emission during room temperature D-desorption from electrolytically loaded Pd:Dx cathodes was also studied. The X-ray emission energy observed was quite similar to the PGD case. However, the intensity in this case was almost 13 orders of magnitude lower due to the much lower deuterium fluxes involved.

1. Introduction Karabut in the LUTCH Laboratory in Russia recently reported X-ray laser (~1.5keV) emission from metal targets such as Ti and Pd, which served as the cathode in a high-current pulsed deuterium glow discharge (PGD) plasma diode. 1 ' 2 Later, he vividly demonstrated the potential capability of this type of laser with a small follow-up 10 W "prototype" unit, which "drilled" a 9 mm diameter hole in a 3 cm thick plastic target. This remarkable unit is more compact and provides a shorter wavelength than any prior "table top" X-ray laser. Staff at the University of Illinois at Urbana-Champaign (UIUC) have undertaken theoretical and experimental studies of the mechanisms involved in this unique X-ray emission phenomenon. 2 ' 3 In UIUC's experiments, it was established that anomalous X-ray emission is observed during PGD operation at a pressure of 0.1-0.5 Torr and at a spacing of about 4.0 mm between the cathode and anode. The current pulses have a square shape 314

315

with 0.2-2.0 ms duration and a rise time of 0.1 /xs. The glow discharge operated at a voltage as low as 300 V with a pulsed current up to 2 A. These crucial conditions are similar to those in Karabut's earlier studies, 1,2 but the voltage operation down to 300 V represents a new region. This paper will briefly describe the UIUC pulsed deuterium bombardment glow discharge project. The X-ray diagnostics employed and their calibration will be discussed. The calibration will be applied to discharge data to determine the power, intensity, dosage, and efficiency of the X-ray observed. Finally a brief discussion is given of related experiments using a deuterium flux created by desorption of D loaded in a Pd target electrolytically. These experiments have much lower D-fluxes than PGD, but low level X-ray production thought to be related to the discharge phenomenon. 2. E x p e r i m e n t a l S e t u p The UIUC staff have designed and fabricated a unique new type of discharge chamber (Fig. 1), which contains a water-cooled cathode (the target can be mounted easily, and is capable of linear motion), a stainless steel anode (capable of angular motion), and a photodiode soft X-ray detector (which will be discussed in-depth shortly). A beryllium filter was placed in front of the detector to prevent detection of visible light. In order to reduce the electrical leakage current between the anode and the ground and to confine the plasma to a smaller volume, a glass tube is added to surround the electrodes, as shown in Fig. 1. On both ends of the tube, plates covered by insulating material are used to provide a sealed boundary for the discharge. Steady state I-V curves obtained after the addition of the glass tube showed that the applied voltage increased by 50%. A hole of 1cm diameter was drilled into one side of the tube to allow X-rays to reach the detector with minimum absorption.

pump Figure 1.

(a)

(b)

Experimental chamber diagram (a) and discharge view showing glass tube (b).

316

3. A X U V D e t e c t o r T h e o r y / O p e r a t i o n The AXUV-100 detector is a silicon p-n junction photodiode that is well suited for the measurement of soft X-rays. Incoming photons or charged particles create electron-hole pairs in the junction of the photodiode. The total number of electronhole pairs generated depends on the materials used in the photodiode and the incoming particle energy. For the AXUV, the average energy for electron-hole pair creation £"e-h is 3.7eV. 4 However, phenomenons that also require some of the incident energy include "dead" doped regions and surface recombination. The percentage of the total incident energy E\ going into electron-hole pairs is the "quantum efficiency" r/Q. Fortunately, the AXUV used has been engineered to approach theoretical quantum efficiency.4 Thus, the number of electron-hole pairs is E\ divided by -Ee-h- The p-n junction of the photodiode sweeps the electrons and holes across the junction and out through contacts. Thus, if the number of electronhole pairs is known, the current they create can be calculated, or vice versa. The measured current production characteristics of the AXUV are shown in Fig. 2. 4 The y-axis of Fig. 2 is the responsivity of the photodiode, which is measured in A/W. With the responsivity information, it is simple to backtrack from the measured current to calculate the power incident on the detector. However, an oscilloscope was used to measure the voltage created. Thus, a basic circuit consisting of the AXUV photodiode and the oscilloscope is needed to understand the measurement (Fig. 3). As seen in Fig. 3, the AXUV photodiode is modeled as a current source accompanied by an inevitable series resistance i?s - due to the silicon that the electrons

Photon energy (eV)

10

0.3

100

1,000

40,00

0.2

iC

0.1

0

'

Photons * " Electrons - Hydrogen ions

'••

100

1,000

10,000

40,000

Electron/hydrogen ion energy (eV) Figure 2.

AXUV photodiode responsivity in amps per watt. 4

317

RS

+

I

~5 Rl

AXUV

Vos

1 M or 50

Oscilloscope Figure 3.

Basic circuit of the AXUV (including a series resistance) and the oscilloscope.

and holes must travel through to escape. The series resistance is assumed to be 5 O.4 The oscilloscope has an input resistance i?i, which can be set at either 1 MO or 50 0. In the AXUV setup, the voltage read by the oscilloscope is Vbs = ^AXUV-RI,

(1)

where /AXUV is the current generated by the AXUV photodiode. The fraction of the total current that this corresponds to is

//AXUV =

Ri + Rsw

(2)

Equations (1) and (2) show that a large input resistance R\ gives a high amplification, hence an accurate reading. However, the photodiode is a capacitive device, and the rise time of its response is directly proportional to the resistance it is discharged over: r = 2.2(i? s + Ri)C,

(3)

where C is the capacitance of the photodiode. 4 The capacitance depends on the detailed photodiode properties, but a 4 pF value is assumed here. The fraction of the measured current and rise time calculation results for the 1 MJ7 oscilloscope input resistance are given in Table 1. As seen, the theoretical rise time for the IMilRi is rather large (/xs). However, the other option, i.e. the 50 il input resistance, reduces the fraction of the total current measured. For the initial experiments here, we elected to use the 1 Mil resistance to retain accuracy while sacrificing to some extent the time resolution. Since the X-ray output measurement duration is in the millisecond range, a rise/fall time of several microseconds should give reasonable detail.

318 Table 1. Current measurement fraction and rise time calculations for the high-oscilloscope input resistance Parameter Series resistance Oscilloscope high-input resistance Photodiode capacitance Fraction of measured current Rise time

Symbol

Units

Value

Rs

Q

5 10 6 4 ~1.00 8.8 x l O " 6

-Rl-High

n

C

pF

fl-lMfl TlMfl

s

4. Calibration The calibration of the AXUV photodiode was done with a 7.5 mCi 14 C source. Carbon-14 is a beta emitter with average beta energy Ep of 49.5 keV.5 Although 14 C is a beta source rather than an X-ray source, responsivity data is available up to 30keV for electrons. While this is 20keV short of Ep, the scale of Fig. 2 is logarithmic, and the electron responsivity slope at the highest graphed energy is nearly flat. Responsivity data from Fig. 2 is extrapolated to the energy of 14 C in Table 2. If the measurement techniques for 14 C are accurate, they should also be accurate for soft X-rays; the only difference being the responsivity of the AXUV. To match the measured results with the source intensity, the power that the 14 C source delivers to the collector must first be calculated: PB = AEpAB-^(W), (4) As where A is the source activity (decays/s), Ep the average beta energy (J), AD the detector surface area (cm 2 ), and Ag is the beta source surface area (cm 2 ). The oscilloscope voltage can then be calculated by VOS = 3 ? C I 4 P D J R I ( V ) ,

(5)

where 5R(^14 is the responsivity of the AXUV for 14 C betas (A/W), P D the power delivered to the detector by the 14 C source (W), and R\ is the input resistance of the oscilloscope (f2). The calculated oscilloscope voltage and associated parameters are given in Table 3 for comparison with measured values cited later. To eliminate background light, the photodiode was placed in a container that blocked out light on all sides but the entrance. The detector head was faced away from the entrance to minimize the light. A 20 MHz low-pass filter was used with Table 2. Electron Ep = 4 9 . 5 k e V 4

responsivity

data

near

Electron energy (keV)

Responsivity (A/W)

15 20 30 50

0.237 0.238 0.240 0.244 (extrapolated)

319

the oscilloscope to reduce the noise to a //V magnitude. The 14 C source was then placed in the container and gently pressed against the detector face. Since the 14 C source completely covered the detector face, essentially no light reached the AXUV. Several consecutive measurements were taken to find a stable, reproducible signal. The final measurement gave a voltage of 2.70 ± 0.25 mV. This result is about a fifth of the projected voltage in Table 3. However, a thin layer of glass covers the 14 C source, and this is thought to attenuate the emitted betas, resulting in the smaller measured voltage. Table 3. Projected oscilloscope voltage Vo s for the 7.5mCi 14 C source Parameter

Symbol

Units

Value

Activity Average beta energy Detector surface area Source surface area Power delivered to the detector Responsivity to 1 4 C betas Projected oscilloscope voltage

A

mCi keV cm 2 cm 2 nW A/W mV

7.5 49.5 1.0 38.3 57.5 0.244 14.0

£/3 AD AS PD

5RC14

vQs

5. Results from A X U V Photodiode X-ray Measurements Representative X-ray power measurements read are shown in Fig. 4. The first "step" in the figure at about 0.04 V is the background signal caused by pickup from the pulsed power supply. The sharp spikes at the beginning and end of the second rise are attributed to the extended rise time of the photodiode (due to the 1 MQ oscilloscope input resistance). The second sharp rise near the middle of the pulse is attributed to the X-ray emission. It demonstrates two very striking features. First is the delay before initiation. Second, as seen later (Fig. 6), the X-ray energy must exceed 600 V (due to the Be filter on the detector). Yet the discharge voltage was only ^300 V. This confirms the very non-linear behavior of this unusual X-ray generation mechanism. 5.1. Solid Angle

Considerations

For the solid angle calculation, it is assumed that the soft X-rays generated are between 0.5 and 2 keV. The average responsivity in this region is about 0.270 A/W. Next, the fraction of the source X-rays that the detector "sees" must be found. The cathode and anode were surrounded by a glass cylinder during the plasma experiment to prevent arcing problems. A hole drilled in one of the vertical sides of the cylinder allowed the X-rays to escape and be collected. A diagram of the glass cylinder/vessel system is shown in Fig. 5. (The geometry leading to this setup is shown in Fig. 1.)

320

The chord subtended by the hole was measured to be 400 mm. Then the total subtended angle #TOT is found to be 1.63 radians. To calculate the surface area of the vessel, hence detector, that this corresponds to, a solid angle surface area equation is used:

de

SA •#TC

2vr

sin(/>d0d6> = r227r( 1 - c o s f - ^ ) )•

(6)

The total angle subtended is divided by two here because the <j> angle is measured from the vertical (z-axis) in the spherical coordinate system. Next, SA can be used

0.20-

p = 500 mTorr

nal (vo

0.15-

0.25

cd c

5 o.io%

0.20 0.15

u> (0 0.10 o 0 05 V, tl)

JU 0.05

8 ^JUUUV\AJU

0.00"

8

0.00 -0.05

0.0&

-0.100.000

Q002

0.000

Time (s)

p = 5 0 0 mTorr •S2.

0.10

">

0.05

!

15 a

0.002

Time(s)

k

0.00

0.05

T i m e (s)

Figure 4. Three measurements of the X-ray emission pulse at 500 mTorr. Measurement 1 is the top left graph, measurement 2 is the top right, and measurement 3 is on the second row.

321

Surface area

Subtended

Hole in glass cylinder

X-ray laser vessel

Figure 5.

Geometry of the glass cylinder /vacuum vessel system.

to calculate the X-ray power at the source by using (7). A beryllium filter was used to prevent transmission of unwanted photons and charged particles to the detector (the detector's transmission curve is shown in Fig. 6). Therefore, a transmission compensation factor is included in the X-ray power calculation. Px-ray = V 0 s ^ ^ — j ~ - ^ S A - J - ( W ) , -Kl «X-ray JF ^-D JE

(7)

where V"os is the voltage read from the oscilloscope (V), R\ the oscilloscope input resistance (0), 3?x-ray the responsivity for the soft X-rays (A/W), / F the average transmission fraction through the Be filter, AD the surface area of the detector face (cm 2 ), SA the surface area subtended by the hole (cm 2 ), and / E is the fraction of X-rays escaping through the hole in the glass cylinder. Note from Fig. 6 that the Be window cuts off all X-rays below 600 V. Thus, as stressed earlier relative to Fig. 4, the observed X-rays must have energies >600V (despite the i 3 and glow discharge 2 Target/Ref.

A£d(lab), (keV)

J (mA)

T (K)

Ue, (eV)

Closest metal-host level

£(level), (eV)

Ti" Ti13 Ti (GD) 2

5-30 2.5-10.0 0.8-2.45

0.054 0.06-0.25 225-450

263 186 >1000

30 6515 610150

Ti(MII/MIII) Ti(MI) Ti(LII)

32.6 58.3 461

The screening potential Ue increases roughly logarithmicly with increase in deuteron current J. The various metal-host (Ti) electron shell energy is consistent with the screening potential values Ue.2

Thus, when the GD low-energy yields are analyzed in the same way as accelerator data, 12,13 they exhibit a larger enhancement at very low D-energy (Ed < 2.45 keV) than was expected from the accelerator bombardment. Further increase in current density (say in TOKAMAK devices) could lead to enormous enhancement of fusion reaction rate in construction metals from which the first wall is built. Note that the enhancement data on tungsten obtained even with low-current accelerator 7 ' n gives high screening potential value Ue = 220 eV. Thus, suggesting same logarithmic

333

dependence of Ue on current density the large enhancemnt of fusion reaction is expected at J ~ 1 A/cm in those construction material. These preliminary GD experiments also showed that Ti-cathode deuteron bombardment in the PGD in is always accompanied by intensive emission of the soft X-ray quanta. In the experiments involving TLD in GD with Ti-cathode at / = 200 mA and U = 1.25 kV, the high intensity (Ix = 10 13 photon/s in 47rsteradian), soft X-ray emission with quanta energy Ex = 1.1-1.4 keV was detected. It is important to note that the mean energy of X-ray photons emission is close to the bombarding deuteron energy. In order to establish the source of the X-rays a special movable design of the anode was employed, such that the anode position could be varied with respect to cathode This allowed runs with a "plasma"-anode (i.e. when the metal anode was shifted 20 mm aside with respect to cathode, Fig. 5a). Then the cathode area was fully opened toward a window viewed by a camera with X-ray film (recall Fig. 1). The X-ray emission image obtained showed a bright spot comparable with diameter of roughly the cathode area. Analysis of measurement with various anode displacements suggests that > 90% of the X-ray emission comes directly from the Ti-cathode surface.The energy of X-ray obtained from Be-shielded TLD measurements was roughly equal to the discharge voltage /deuteron energy in the range of 1.2-1.8 kV at constant discharge current J = 200 mA. To change the discharge voltage at constant current, the deuterium pressure was varied over 2.0-9.0 mmHg. At U < 1.6 kV, the X-ray quanta energy is about Ex = 1.30 ± 0.15 keV independent of the voltage applied, while at U > 1.6 kV the X-ray energy slowly increases with voltage, reaching Ex = 1.43 ± 0.15 keV.

(a)

(b)

Figure 5. (a)- X-ray image of the Ti-cathode using the pin-hole camera. The objective of 0.3 mm diameter is narrowed by use of a 15 (im Be shield in front of the camera. The image is a positive imprint, (b) - Correlation between X-ray and current pulses in GD (Ix ~ 10 1 4 . 1.5 keV).

334

The X-ray yield per deuteron increases exponentially with the applied deuteron current at E& ~ 1.5-2.0 keV as it is shown in Fig. 6

X-ray yield per deuteron versus effective 4.00E 04

power at p = 4.2 mm

3.50E 04 3.00E 04

^=0.977

2.50E-04 2.00E-04 1.50E-04 1.00E-04 5.00E 05 COOEiOO 40

Power p* (W)

Figure 6. Yield of X-ray quanta per bombarding deuteron from the Ti-cathode versus effective discharge power at p — 4.2 torr.

The results obtained in experiments with glow discharge suggest nonnegligible edge plasma effects in the ITER TOKAMAK that were previously ignored. In the case of the ITER DT plasma core, it is possible to estimate the DT reaction yield at the metal edge due to plasma ion bombardment of the loaded first wall and/or divertor material. Then the yield of 3.6 MeV alpha-emission (DT reaction charged product) near the surface of the wall would be enhanced during the metal bombardment (e.g. W as a divertor material) similarly to DD-reaction GD studies. This estimate indicates that during one year of ITER operation (maximal power deposition up to P ~ 0.1 GW/m 2 8 ) , about 1014 c m - 2 He4 atoms (formed from the stopped 3.6 MeV alpha particles) would be stored within the near surface metal (tungsten) layer of ~ 6 jiva depth. The helium atoms will be precipitated at dislocation cores or captured in dislocation atmospheres (Cottrell atmosphere) and serve as an obstacle with respect to dislocations motion. Thus, the helium capture could induce a micro crack formation at the metal surface caused by reduction of plasticity due to the decreased dislocation mobility. The first wall erosion by sputtering caused by low-energy d, t and He ion bombardment would be also enhanced by intense soft X-ray quanta during the bombardment of the wall by keV deuterons. This effect is expected due to full deposition of X-ray quanta energy in the thin layer of the wall. In this connection, the high current glow discharge could be considered as an ideal instrument for simulation of the plasma edge effects at the metal surface. Experiments performed with metals serving as construction materials of first wall

335 of I T E R would provide necessary information on DD and D T reaction enhancement and emission of accompanied intensive X-ray q u a n t a caused an excessive helium storage and radiation stimulated corrosion near their surface layers. 1 6 4.

Conclusions • At Ja > 1.0 A / c m 2 and E& ~ l - 2 k e V , the total yield of DT-reaction (scaled to GD with Ti target) for ~ 10 years of operation is found to be ~ 10 1 4 H e ~ 4 atoms, stopped at depth ~ 5.0 m m from the surface. This corresponds to ~ 10 1 7 c m ~ 3 H e - 4 concentration beneath the surface. • T h e 4 He-atoms will be precipitated along dislocations or captured in metal vacancies serving as obstacles for dislocation motion resulting in additional stress. • Reduction in plasticity (e.g. in W ) due to the He capture is caused a microcrack generation at the near-the surface layer and fracture of the first wall. • Intense soft X-ray emission at the surface may also enhance erosion/sputtering process at the surface of the first wall caused by X-ray energy deposition in the near-the-surface layer during charged particle bombardment. • T h e edge plasma effects at the first wall, including blistering, cracking and erosion, would be significantly underestimated because the enhancement of D D / D T reaction and accompanying radiation processes at very low deuteron energy are neglected. • T h e high current pulsed GD testing appropriate cathode materials (W, St. steel) could be a suitable instrument to simulate edge plasma effects at ITER'S first wall.

References 1. 2. 3. 4. 5. 6. 7. 8. 9. 10. 11. 12. 13. 14. 15. 16.

H.S. Bosch and G.M. Halle, Nucl. Fusion 32, 611-631 (1992). A.G. Lipson, A.S. Roussetski, A.B. Karabut, and G.H. Miley, JETP 100, 1175 (2005). M. Junker, A. D'Alessandro, S. Zavatarelli et al, Phys. Rev. C57, 2700 (1998). M. Aliotta, F. Raiola, G. Gyurky et al, Nucl. Phys. A690, 790 (2001). K. Czerski, A. Hulke, A. Biller et al, Europhys. Lett. 54, 449 (2001). F. Raiola, P. Migliardi, G. Gyurky et al, Eur. Phys. J. A13, 377 (2002). F. Raiola, P. Migliardi, L. Gang et al, Phys. Lett. B547, 193 (2002). D. Reiter, Edge plasma physics overview, Trans. Fusion Tech. 33, 249 (1998). V. Violante, A. Torre, G. Silvaggi, and G.H. Miley, Fusion Tech. 39, 266 (2001). U. Greife, F. Gorris, M. Junker et al, Z. Phys. A465, 150 (1995). F. Raiola et al. (LUNA collaboration), Electron screening in d(d,p)t for deuterated metals, Nucl. Phys. A719, 61C (2003). H. Yuki, J. Kasagi, A.G. Lipson et al, JETP Lett. 68(11), 785 (1998). J. Kasagi, H.Yuki, T. Baba et al., J. Phys. Soc. Jpn. 71(12), 2881 (2002). K. Eder, D. Semard, P. Bauer et al, Phys. Rev. Lett. 79, 4112 (1997). S.P. Moller, A. Csete, T. Ichioka et al, Phys. Rev. Lett. 88, 193201 (2002). For He-4 blistering in ITER first wall see: Fusion Sci. Tech. 47 (4), 821-1295 (2005).

G E N E R A T I O N OF D D - R E A C T I O N S IN A F E R R O E L E C T R I C K D 2 P 0 4 SINGLE CRYSTAL D U R I N G TRANSITION T H R O U G H C U R I E P O I N T (Tc = 220 K) A.G. L I P S O N A N D G.H. M I L E Y Department

of Nuclear, Plasma and Radiological Engineering, Urbana- Champaign, Urbana, IL 61801, E-mail: lipson@uiuc. edu

University USA

of Illinois

at

A.S. R O U S S E T S K I Lebedev Physics

Institute,

The Russian

Academy

of Sciences,

Moscow

117285,

Russia

A.G. L I P S O N A N D E.I. S A U N I N Institute

of Physical

Chemistry, The Russian Academy Moscow 117915, Russia

of

Sciences,

A new approach to develop a source of 2.45 MeV neutrons caused by polarization reversal in KD2PO4 single crystal (DKDP) during its passage through the Curie point (T c = 220 K) is presented. The background of this approach is referred to observation of neutron/proton emission in DKDP during paraelectric-ferroelectric phase transition to spontaneous polarization state (and vise versa) upon the heating/cooling of crystal through Curie point Tc = 220 K. The proposed source is based on earlier established proof of deuteron acceleration and neutron generation in the crystalline lattice of ferroelectrics during their transition to spontaneously polarized state (polarization reversal). In order to obtain neutron yield for practical application, the proposed solution foresees a separate DKDP crystals serving as cathode and anode and undergo to simultaneous ferroelectric phase transition in low-pressure deuterium atmosphere.

1. Introduction Naranjo et al.1 presented a desktop neutron generator based on deuteron beam ionized and accelerated up to 100 keV by electric field arising from the spontaneous polarization of ferro/pyroelectric LiTa03 crystal at a low-pressure deuterium gas adsorption in their Letter to Nature. The results of this work are appeared to be solid with respect to both experimental and theoretical aspects of 2.45 MeV DDneutron production. However, a certain early history exists on a deuteron fusion driven by a strong crystalline electric field. The fracto-fusion caused by a weak neutron emission has been observed during the fracture of deuterated dielectric crystals (i.e., induced polarization), where cracks serve as tiny accelerators. 2,3 Such crack propagation in crystalline dielectrics is accompanied by high-energy electron and X-ray emissions up to 100 keV (see Refs. 2, 3 and references therein), similarly to that emitted by pyroelectrics with 336

337

a large spontaneous polarization. l The secondary deuterons generated by fast electron emission can be accelerated up to keV energy range inside this cracks by a strong electric field (>10 8 V/m) released on the rapture of chemical bonds in these crystals. The DD-reaction in such crack is prompted by deuteron bombardment of "deuterated target" (i.e. crack's wall surface). The idea to use spontaneous polarization in deuterated ferroelectrics to obtain DD-fusion was first explored at the Institute of Physical Chemistry, The Russian Academy of Sciences, Moscow. 4 ' 5 The reason was a strongest electric field in the lattice (E ~ 1010 V/m) that arises in the course of spontaneous polarization during heating or cooling of KD2PO4 (DKDP) single crystal through the Curie point Tc = 222 K (i.e., exactly the same presupposition that is considered in Ref. 1, when explaining benefits of the spontaneous polarization for deuteron acceleration). In these articles, the neutron emission has been detected during DKDP crystal passage through the Curie point resulting in spontaneous polarization. KH2PO4 (KDP) single crystal (similar to DKDP one, but containing just hydrogen, instead) did not demonstrate neutron emission above the background level during transition through its particular Curie point (Tc = 123K due to isotopic effect.). In contrast to Ref. 1, in the prior experiments 4 ' 5 a deuterium atmosphere was not used because the hostdeuterium in ionic form is presented in the lattice. In such a case, the DKDP crystal serves both as a source of accelerated deuterons (suggesting no need for their field ionization) and the deuterated target, simultaneously. These DKDP crystals have generated reproducible neutron emission, though three orders of magnitude lower than that in Ref. 1. The cause of a high-neutron yield in Ref. 1 is referred to both full deuterium ionization provided by tungsten tip and deuteron source-target separation, resulting in significantly higher D + energy and current compared to those inside the cracks. Furthermore, later a team from Tokyo Metropolitan University, inspired by fracto-fusion works, 2_5 performed experiment on neutron generation during the fracture of piezoelectric LiNbC>3 crystals (with the structure similar to that of the LiTaOs) in a D2 atmosphere with pressure p > 30kPa. 6 ' 7 In this particular experiment, the ionization of deuterium gas occurred at the surface of the charged piezoelectric particles, similarly to Ref. 1, so the source of deuterium was a D 2 gas. Since the surface of the LiNb0 3 particles with adsorbed deuterium served as a neutron target (contrary to the separate ErD3 target in Ref. 1), the detected neutron yield was also much lower than that obtained by Naranjo et al. Here we demonstrate our results on DD-reaction (neutrons and tritium) in DKDP during transition through Curie point that are enhanced by recent measurements of in situ 3MeV proton emission using CR-39 track detectors. We also discuss a new approach to develop a source of 2.45 MeV neutrons caused by polarization reversal in K D 2 P 0 4 single crystal (DKDP) during its passage through the Curie point (Tc = 220K).

338

2. Experimental • Transitions of KD2PO4 (98% D purity) single crystals through Curie point Tc = 220 K by heating-cooling cycle using LN2 cryostate. Control of transition with thermally stimulated depolarization (TSD). • Neutron measurements with BF3 - seven counter proportional neutron detector. • Tritium measurements with liquid scintillator technique with dissolving of DKDP crystals in H 2 0 . • Recently done: 3.0 MeV proton measurement with CR-39 (open and filtered with Al foils) attached to DKDP plates cycled through Curie point. 3. Experimental Results The amplitude-differential spectra of neutron emission are presented in Fig. 1. As seen, the sum of spectra for DKDP exposed at the neutron detector during ferroelectric phase transition near 220 K are in good agreement with Cf-252 amplitude spectrum. 800

a

700

u,

600

'c

500

g

O

400 30

°"

-

200"

•g

100-

2 50 • 40

b

30 20 10 5

10

15

20

25

30

cChannel Figure 1. Distributiion of the pulses arriving at the neutron detector channels of the pulse height analyzer, (a) From the Cf252 neutron source; (b) during temprature cycling of DKDP crystals near T c .

This picture unambiguously confirms presence of neutron emission during transition through Curie point. The neutron counts are consistent with spontaneous polarization occurring in DKDP crystals during ferroelectric phase transition as it is shown in Fig. 2. Parameters of neutron emission, including flux intensity in DKDP crystals near T c , in comparison with KDP and those obtained outside the Tc temperature interval are shown in Table 1.

339

0

o 1 3 -2

220

221

222

223

7"(K)

Figure 2. (a) Spectrum of thermal depolarization during the heating of DKDP sample near T c ; (b) corresponding histograms of neutron bursts. Here L, a is the confidence level of the observed neutron bursts, and Nb is the average background level.

As seen from Table 1, the neutron emission is occurred only in DKDP crystals (not in KDP) and strictly in the temperature range corresponding to spontaneous polarization (219-223K). Generation of DD-reaction in DKDP crystals during transition through Curie point is confirmed by measurement of 3.0 MeV protons emission (d(d, p)t reaction) during similar transitions (Fig. 3). Tritium concentration in DKDP has been measured by liquid scintillation technique. The samples were 100 times cycled through Curie point in a glass capsule. After the cycling the crystals, glass, and gas atmosphere of the ampule were analyzed. The results (in units of 109 T-atoms per gram of DKDP) are presented in Table 2.

Table 1. Parameters of neutron emission in KH2PO4 and KD2PO4 single crystals in various temperature intervals Crystal

KH2PO4 KH2PO4 KD2PO4 KD2PO4 KD2PO4 KD2PO4

(m (m (m (m (m (m

= = = = = =

0.8j 0.8f 0.8| 0.5j 0.81 0.8 j

Temperature interval: A T (K)

Foreground— background (cps)

Neutron emission n (n/s)

121-125 219-223 210-215 219-223 219-223 221.0 ± 0 . 5 ; 222.0 ± 0 . 5

0.000 0.001 0.001 0.012 0.020 0.025

0.40 ± 0 . 1 3 0.61 ± 0 . 1 6 0.75 ± 0 . 1 5

±0.005 ± 0.005 ±0.005 ±0.004 ± 0.004 ± 0.004

340

open CR-39 11 mAI/CR-39 44 mAI/CR-39

3.0 ± 0.2 MeV

18

2.75 ± 0.25 MeV

•f12j

1.85 ±0.30 MeV

S 107*5

8-

"

64

20

4,8

5,0

Jj 52

5,4

5,6

5,{

J 6,0

62

Track diameter (m) Figure 3. Three MeV proton emission: 40 transitions through Curie point in a row with attached open and filtered CR-39 detectors: the detected track diameters are consistent with 3 MeV proton energy losses in Al foils.8

Neutron and proton emission yields per transition through Curie point: • Neutron yield from d(d, n)He 3 reaction was found to be Y„ = 20 ± 4 (n/transition-g) in the range of 219-223 K. • Branching ratio between neutrons and tritium should be: Y„/Yt ~ 10 . • Recently measured (with CR-39) 3.0 MeV proton yield from d(d,p)t reaction, taking into account efficiency of CR-39 detection of 3.0 MeV protons (e p = 0.076) at (Np) = 0.5 ± 0.1 count per transition was found to be y p = 12 ± 3 (p/transition-g). Thus, there is no significant difference between DD-reaction channels when 3.0 MeV proton and neutron yields are compared. That is why, the seven order

Table 2. Tritium concentration measurements by liquid scintillator technique (in units of 109 T-atoms per gram of DKDP) # Sample

DKDP crystal

Cell glass

Cell atmosphere

Total

Control 100 cycles through T c

5.0 ± 0.2 5.9 ± 1.1

8.3 ± 1 . 3

9.2 ± 1 . 5

5.0 ± 0.2 23.4 ± 1 . 8

*The DKDP sample m = 0.5 g was subjected to 100 heating-cooling cycles in isolated glass cell at atmospheric pressure. Accordingly to this measurement the yield of tritium was found to be Yt = (1.82 ± 0.25) x 10 8 (t/transition).

341

enhancement of tritium channel compared to neutron and proton yield observed during DKDP cycling through Curie point cannot be explained by conventional DD-reaction. 4. Novel Neutron Source based on Ferroelectric Transition in DKDP Taking into account both results of works, 1 ' 4 , 5 we are presenting novel type of neutron source based on transition of DKDP single crystal through Curie point at Tc = 220 K (polarization reversal) and employed on principles of a high-voltage glow discharge in a low-pressure deuterium atmosphere (Fig. 4). In order to increase deuteron kinetic energy, the "paired DKDP crystal system" suggesting both ferroelectric electrode pair 9 operating as cathode and anode is proposed. The polarization reversal in both single crystal DKDP cathode (having a conic shape) and rounded shape anode separated by a spacing of ~ 1 cm is caused by heating/cooling through the Tc = 220 K. To this goal, both cathode and anode inserted inside metallic Cu frames that are attached with the dielectric epoxy composition to the cryostat wall. The liquid nitrogen (LN) cryostat is supplied with a heater allowing change in DKDP temperature near 220 K. In order to keep a constant positive electric charge at the cathode surface, the back face of the DKDP cathode is grounded via an ohmic contact (silver film) sputtered on top of the crystal attached to the epoxy layer. To keep negative electric charge at the surface of the anodic DKDP piece, a small positive potential is applied to its back face. The sealed cryostat chamber is filled with D2 gas at pressure about 10 mTorr. During simultaneous transition through Curie point both cathode and anode are triggered to a spontaneous polarization state. In such a case, the strength of electric field in the gap between their surface would reach a value E ~ 108 V/cm due to a large value of spontaneous polarization in DKDP (P s ~ 5.0 x 10~ 6 C/cm 2 ). This electric field will stimulate an intensive field emission of energetic electrons (up to hundreds keV range) from the cathode surface and X-ray generation during anode electron bombardment. The electron emission will produce mostly secondary D + ions from the anode because the binding energy of deuterons in DKDP lattice is very small (hydrogen bonds). The deuterons escaping from the anode will be accelerated in the electrostatic field in the interelectrode gap toward the surface of DKDP cathode and bombard it with energy about 100 keV in the laboratory system. At realistic time of the passage through Tc chosen as ~ 10s (e.g., AT = 222-220K and AT /At ~ 0.2 K/s, comparable with Ref. 5), the expected electron current density would be J e ~ 1.0/xA/cm2. Assuming a secondary ion emission coefficient ~ 1 and taking into account possibility of direct deuteron field emission from the DKDP anode tip, we suppose that the D+ current density would be the same order of magnitude as an electron emission one. Thus, at -Ed ~ 100 keV and Ja ~ 1/xA/cm2, the expected neutron yield can be estimated as 10 5 -10 6 n/s in AIT ster. Notice that the deuterons escaping from the anode surface would be fully substituted by deuterium ion adsorption at the DKDP surface and its ferroelectric properties could be

342

recovered, resulting in multiple usage of the source (passage through Tc) to generate neutrons. The proposed neutron source can be further modified resulting in production of enhanced stationary neutron yield by application of pulsed voltage (several kV) between cathode and anode at constant temperature T < Tc (e.g. T = 77 K). This application provides polarization reversal at spontaneously polarized ferroelectric state by triggering electric dipole moment orientation by AC electric field.

Figure 4. Diagram of cryo-set up of 2.45 MeV neutron source based on a high-voltage discharge between DKDP single crystalline cathode and anode during their passage through Curie point. 1 0

5. Conclusions Generation of DD-reaction resulting in neutron and 3 MeV proton emissions in DKDP ferroelectric crystal during passage through Curie point has been established. It was shown that neutron and proton channels in DKDP crystal give comparable nuclear yields. Large amount of tritium production ( ~ 2 x 10 8 T 3 at./transition) cannot be referred to usual DD-reaction. The factor of spatial separation of deuteron source and target in deuterated ferroelectrics can be used to obtain large neutron yield during transition of these ferroelectrics to spontaneously polarized state. New type of neutron source based on electric discharge between two ferroelectric KD2PO4 (DKDP) crystals during their polarization reversal at T = 220 K in D2/T2 atmosphere is proposed. No high voltage power supply. Small size. Projected intensity Yn = 10 6 (D 2 )-10 8 (T 2 ) n/s. Potential applications include Homeland security and oil exploration as a borehole source.

343

References 1. B. Naranjo, J.K. Gimzewski, and S. Putterman, Nature 434, 1115-1117 (2005). 2. V.A. Klyuev, A.G. Lipson, B.V. Deryagin et al, Sov. Tech. Phys. Lett. 12 551-555 (1986). 3. B.V. Deryaguin, A.G. Lipson, V.A. Kluev et al., Nature 341, 492 (1989). 4. A.G. Lipson, D.M. Sakov, V.B. Kalinin, and B.V. Deryaguin, Sov. Tech. Phys. Lett. 18, 90-95 (1992). 5. A.G. Lipson, D.M. Sakov, E.I. Saunin et al, JETP 76(6), 1070-1076 (1993). 6. M. Chiba et al, Nuovo Cimento A108(10), 1277-1280 (1995). 7. M. Fuji et al, Jpn. J. Appl. Phys., 41(4A), 2115-2119 (2002). 8. A. G. Lipson et al., Proc ICCF-10 (Boston, MS, 2003). 9. J.A. Geuther and Y. Danon, J. Appl. Phys., 97, 074109 (2005). 10. A.G. Lipson and G.H. Miley, A novel portable ferroelectric source of fast MeV neutrons for homeland security applications. Transactions of American Nuclear Society, 2006 (in press).

S T U D Y OF ENERGETIC A N D T E M P O R A L CHARACTERISTICS OF X - R A Y EMISSION F R O M SOLID-STATE C A T H O D E M E D I U M OF H I G H - C U R R E N T GLOW DISCHARGE

A.B. K A R A B U T FSUE

"LUCH"

24 Zheleznodorozhnaya St, Podolsk, Moscow E-mail: [email protected]

Region

14-2100,

Russia

Experimental results on X-ray emission characteristics from the cathode material in the high-current Glow Discharge (GD) are presented. The X-ray emission ranging 0.6-6.0 keV and more with the dose rate up to 0.01 J / s has been registered. Two emission modes were obtained in the experiments: (1) diffusion X-rays were observed as separate X-ray bursts (up to 5 x 1 0 s bursts a second and up to 10 6 X-ray quanta in a burst); (2) X-rays in the form of laser micro-beams were registered (up to 10 4 beams per second and up to 10 1 0 X-ray of quanta in a beam, angular divergence being up to 1 0 - 4 , the duration of separate laser beam about T = 3 X 1 0 ~ 1 3 - 3 X 10~ 1 4 s, the estimated separate beam power of 10 7 -10 8 W). The emission of the X-ray laser beams occurred during the GD operation, and, after the GD current switch off.

1. Introduction Experiments aimed at illuminating the anomalous high-energy phenomena in the solid-state cathode medium of the high-current glow-discharge were carried out for years. Earlier experimental results showed that the character of detected X-ray emission was essentially different from the known X-ray emission types. 2. Experimental Method and Results The experiments were carried out using a high-current glow discharge device (GDD) in deuterium, hydrogen, Ar, Kr, and Xe. The GDD operated on a pulse-periodic power. The power supply produced direct pulse-periodic current of rectangular shape of pulse. In the separate experiments the pulses duration were from 0.1 ms up to 1.0 ms, the period was from 0.3 ms up to 100 ms. The GD conditions were following: current (amplitude) was from 30 mA up to 200 mA, voltage 1300-2300 V, a gas pressure in the discharge chamber was 3-10 Torr. The X-ray emission registration was carried out by thermo-luminescent detectors, X-ray pinhole, and scintillation detectors with photomultiplier. The energy spectrum of the X-ray emission was registered with the help of a curved mica crystal spectrometer. The cathode samples made of Pd and other metals were placed on a cathode-holder above which a window for output penetrating radiation was provided. 344

345

The window was shielded by 15/im-thick Be foil for protecting the detectors from visual and ultraviolet radiation. Various detectors were installed by the window to measure the output penetrating radiation (Fig. 1). To estimate the intensity and evaluate the mean energy of the soft X-ray emission in the GD, thermo-luminescent detectors (TLD) based on crystalline AI2O3 and, covered by Be foils of varying thickness were used. The temporal characteristics of the penetrating radiation were determined with the help of scintillation detectors with the photomultipliers (PM). Two modes of radiation emission were observed in the experiments: (1) diffusion X-ray emission (Fig. 2) and X-ray emission in the form of laser beams (Fig. 3). The diffusion X-ray emission occurs mainly during the current running in the form of flashes and conforming to the law 1/r2. The value of X-ray emission energy was estimated for the experiments with using system scintillator- PM and the beryllium foil shields for the foil with thickness of 15 and 30/um (Fig. 2a and b). 8 Be =15-300um 9 view A *

A s

-

Figure 1. Schematic representation of an experiment, (a) pinhole, (b) TLD detectors and absorbing Be screens of various thickness, (c) PM-scintillator system, and (d) X-ray spectrometer. (1) Cathode sample; (2) anode; (3) discharge chamber, (4) Be foil screens; (5) X-ray output channel, (6) pinhole objective, (7) X-ray film, (8) absorbing Be foil screens with thickness ranging 15-300 lira, (9) TLD detectors, (10) absorbing Be foil screens for scintillator, (11) scintillator, (12) photomultiplier, and (13) mica crystal spectrometer.

By using the PM scintillation detector the relative intensity of the X-rays was determined as the total sum of the amplitudes HAH a n d H,A2j of all the X-ray bursts within the time interval of 1 second (Fig. 2a and b). The experiments using the scintillator - PM measurement system, and, 15 and 30 /xm-thick Be foil shields allowed to evaluate of the X-ray energy value as J5x- ra y ~ 1.3-2.5 keV (for different cathode materials). Then the relative intensity was reduced to a physical magnitude by the intensity value measured with the TLD detectors (.Ex-ray ~ 1.5-1.8 keV). The generation of X-ray emission in the form of laser beams and began when the GD operational parameters increased (duration of current pulses, current density, GD voltage) and was observed as powerful flashes. The production of X-ray laser beams occurred in pulse-periodic GD some time after ( A T delay time) the GD current pulse trailing. The temporal spectrum of the X-ray emission made up a

346

correlation: the quantity of pulses per a T period of time (T stands for the time period between the GD current pulses) versus the time period between the current trailing edge and the X-ray pulse leading edge. The temporal spectra are discrete in character, consisting of separate lines. The specific pattern of each spectrum is dependent upon the cathode material used. The secondary penetrating radiation (in the form of bursts of fast electrons with small angular divergence) occurred when the targets made of different materials were exposed to X-ray laser beams. The generation of electron bursts was observed in the experiment when the primary X-ray beams passed through Pb targets (of up to 3 mm thickness). Presumably, some multi-photon processes were initiated.

/(mA) 200

Figure 2. The typical oscillograms of the X-ray emission signal from the system PM -scintillator covered with the Be foil with the different thicknes: (a) with covered the 15 /^m Be shield and (b) with covered the 30/im Be shield. The system Pd—D2, the discharge current — 150 mA.

The X-ray emission spectra were measured using the curved mica crystal (50 mm diameter) X-ray spectrometer, the spectrum being recorded on an X-ray film (Fig. 4). Reflection and refraction spectra were registered in the experiment. Reflection spectra being used for data processing. The wave length and the energy of the X-ray were determined according to the expression The energy of the X-ray mX = 2dsin 0;

EX-ra,y = 1.235/A,

where m is the spectrum order, A stands for the X-ray emission wave length in nm, 2d is the constant of the mica crystal lattice (2d = 2.0 nm), and 6 represents the reflection angle. The spectra were repeatedly recorded during the GD operation and after the GD current switch off (for up to 20 h afterward). The spectra pattern

347

includes bands, dark and light spots (consisting of multiple tiny dark and light dots) and separate dark and light small spots. The bands and spots were located in spectral areas specific for a given cathode material used (Fig. 4). The registered energy of the X-ray emission bands and spots (the energetic position of the bands and spots within the spectrum) was dependent upon the cathode material used. The registered X-ray spectra in experiments was similar to characteristic X-ray spectra. It was assumed that the diffusion component of the X-ray emission was registered on the spectrum as a series of bands.

/x-ray,

photons/beam

1.2x1( Pd-D

0.8 x10s 0.4X10B

0 /(mA) 100 0 /x-ray, photons/beam 1.2x1080.8x10s

Pd-Xe

0.4 x10s 0 /(mA)t 100

/v. Photons/beam

/x- ray,

1.2x108 Pd-Kr

0.8x108 0.4x108 0 /(mA) . 100

-•• u4

o --

;

: ml;

Af=100us-«-l—i—

30401-35;

mZ

f(ns)

Figure 3. The typical oscillograms of bursts from X-ray laser beams (PM—scintillator) in the discharge for different kind of gases. The cathode sample is Pd, current: 50 mA. *The pulse peak was cut a discriminator of amplifier, (a) D2, (b) Xe, and (c) Kr.

The X-ray emission bands energy do not correlated with L, M energy of the electron levels (Fig. 4). The laser beams were recorded as dark spots and in case of the emission beam high density they assumed white color (solarization of the photoemulsion) (Fig. 5bd). In certain experiments radiation and thermal destruction of the X-ray film was observed (Fig. 5a).

348

8

*10 54 3

10 54 3 2.5-2 9keV

2.0 1.1-1.3keV _

2.0

10 54 3

2.0

10 54 3

2.0

1.0Q.< , 0.82-0.86keV

1.0 0.9

A

(^X-rayl)

,-J .3-1.5keV

B

0.8

0.7 0.68 0.66

^ 0.81-0.84keV

C

1.0 0.9 ,-,1.35-1.75 keV

0.8

0.7 0.68 0.66

1.0 0.9

0.8

0.7 0.68 0.66

^,1.2-1.8 keV

„

12 3 4 I i- -J 10 54 3

8 2.0

10

12

14

1.0 0.9

1€ 0.8

17

16

^X-ray

(A)

0.7 0.68 0.66

Figure 4. X-ray reflection spectra. Voltage GD: 2350 V, Current: 150 mA. Exposition time 18 000 s (a) X-ray spectrometer measurement diagram; (1) Cathode, (2) Be shield, (3) X-ray cathode emission, (4) spectrometer chamber, (5) slit, (6) curved mica crystal, (7) X-ray film, spectrometer, slit, (8, 9) reflected spectrum X-ray, (10) reflection spectra area, (b) Spectrum of Al-D Glow Discharge system, (c) Ni-D, (d) V-D, (e) Pd-D, (f) Mo-D, and (g) Ta-D.

349

3. Discussion Presumably, some long-lived excited levels with energies up to several keV are formed in the cathode solid-state medium when its surface is exposed bombardment

E E o

• T ^ ^ * *

1 - 2 9.0

8.5

8.0

^X-ray (A)

1.6

1.4

1.5

^x-ray(keV)

m

E. E • in

d

4

. 100 meV) resulting in a most effective lattice-nuclei energy transfer.

• Metallic H/D superfluid25 suggests dramatic enhancement of quantum entanglement between deuterons at those sites Acknowledgments This work was partially supported by the NSF under Grant No. DMR-9982520 and by New York Community Trust. The magnetic property measurements were performed at the Frederick Seitz Material Research Laboratory at UIUC supported by the U.S. Department of Energy under Grant No. DEFG02-91-ER45439. The authors would like to thank Dr. A. Bezryadin (UIUC) and Dr. R. Prozorov (University of South Carolina) for useful comments. References 1. 2. 3. 4. 5.

N.W. Ashcroft, Phys. Rev. Lett. 92, 187002 (2004). B.J. Heuser and J.S. King, J. Alloys Compd. 261, 225 (1997). B.J. Heuser and J.S. King, Metal. Mater. Trans A 29, 1594 (1998). M. Maxelon et al., Acta Mater. 49, 2625 (2001). R. Kirchheim, Acta Metall. 29, 845 (1981).

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6. A.G. Lipson et al, Phys. Lett. A 339, 414 (2005). 7. G. Elsasser et at, J. Phys.: Cond. Matter. 4, 5207 (1992). 8. B. Strizker and H. Wuhl, in: Hydrogen in Metals II. Topics in Applied Physics, v. 29, Ed., G. Alefeld and J. Volkel, Springer Verlag, Berlin (1978). 9. L. Schlapbach, I. Anderson, and J.P. Burger, in Material Science and Tech., v.3B Part II, ed. K.H. Jurgen Buschow, p.287, Weinheim, New York (1994). 10. J. Miller and C.B. Satterthwaite, Phys. Rev. Lett. 34, 144 (1975). 11. J.E. Schriber and C.J.M. Northrup Jr., Phys. Rev. B 10, 3818 (1974). 12. D. Wang et al., J. Alloys Compd. 348, 119 (2003). 13. G.F.J. Garlick and A.F. Gibson, Proc. R. Soc. Lond. Sect. A 60, 574 (1948). 14. B.J. Heuser, G.S. Danagoulian, and A. Lipson (to be published). 15. N.E. Alekseevskii et al, Physica B 163, 659 (1990). 16. A.A. Abrikosov, Phys. Rev. B 64, 104521 (2001). 17. P.M. Grant et al, Phys. Rev. Lett. 58, 2482 (1987). 18. C. Panagopoulos et at, Phys. Rev. B 69, 144508 (2004). 19. H.C. Jamieson and F.D. Manchester, J. Phys. F: Metal Phys. 2, 323 (1972). 20. M. Tinkham, Introduction to Superconductivity, 2nd Ed., McGraw-Hill, 1996, NY. 21. W.L. McMillan, Phys. Rev. 167, 331 (1968). 22. J.M. Rowe et al, Phys. Rev. Lett. 57, 2955 (1986). 23. A.G. Lipson, et al, Phys. Rev. B 72, 212507 (2005). 24. A. Takahashi, Proc ICCF 11 (Marseille, France, 2004). 25. E. Babaev, A. Sudbo, and N.W. Ashcrof, Phys. Rev. Lett. 95, 105301 (2005).

N E W P R O C E D U R E S TO M A K E ACTIVE, FRACTAL-LIKE SURFACES ON THIN Pd WIRES

F R A N C E S C O C E L A N I , A. S P A L L O N E , E. R I G H I , G. T R E N T A , G. D ' A G O S T A R O , P. Q U E R C I A , V. A N D R E A S S I , A N D O. G I A C I N T I INFN-LNF

Via E. Fermi 40, 00044 Frascati (Rome), E-mail: [email protected]

Italy

P. M A R I N I , V. DI S T E F A N O , M. N A K A M U R A , F . T O D A R E L L O , A N D E. P U R C H I EURESYS,

Via hero 30, 00129 Rome,

Italy

A. M A N C I N I ORIM

SpA,

Via Concordia

65, 62100 Piediripa

(Macerata),

Italy

P. G. S O N A Via S. Carlo 12, 20090 Segrate

(Milan),

Italy

F . F O N T A N A , L. G A M B E R A L E , A N D D. G A R B E L L I Pirelli Labs SpA,

Viale Sarca 222, 20126 Milan,

Italy

E. C E L I A , F . F A L C I O N I , M. M A R C H E S I N I , A N D E. N O V A R O CSM SpA,

Via di Castel Romano

100, 00129 Rome,

Italy

U. M A S T R O M A T T E O ST Microelectronics

SpA,

Via Tolomeo

1, 20010 Cornaredo,

Italy

In the framework of anomalous effects coming out because very close interaction of some specific gas [usually Deuterium (D), some times hydrogen (H)] with some specific solid materials [usually Palladium (Pd), some times Nickel or others] is an emerging evidence that the physical condition at the surface of the host element play a crucial role. It has been experimentally demonstrated, by Yoshiaki Arata at Osaka University, that nano-particles of Pd, embedded in a matrix of Zr02, are able to absorb extremely large amounts of H and/or D, at even room temperature and pressure. Because of such results, we re-analyzed some of our previous experiments under the new point of view and were convinced that most of our "positive" results in Condensed Matter Nuclear Science come because of lucky, specific condition of our Pd cathode. We decided to improve the quality of Pd, from the point of view of production of nanostructure at its surface as large (and stable) as possible, in a controllable way, using both electrolytic procedure and special preparation of Pd before the use. Some of our efforts seemed to give positive results, although the stability at long time as to be improved. 377

378

1. Introduction In the framework of Condensed Matter Nuclear Science, it has been recently shown, by Yoshiaki Arata at Osaka University,1 that nano-structures of metallic palladium, stabilized in a matrix of ZrC>2, can rapidly absorb surprisingly large amount of H 2 or D 2 . According to Arata's results and to the Akito Takahashi2 theoretical model, atomic ratios (H, D)/Pd ;§> 1 can be easily accomplished at a pressure of only a few bars into Pd nano-particles, stabilized in a Z r 0 2 matrix. In the Arata's experiments, together with the abnormally high D/Pd ratios, a remarkable excess heat and production of 4 He were detected. On the basis of such results (and new deeper interpretation of some of our previous experimental results 3 that, although quite interesting from the point of view of experimental effects, did not get at that time a satisfactory explanation), we are now convinced that most of the high loading ratios (H-D/Pd) and/or anomalous effects, both thermal and nuclear (by using D), obtained (generally in a not reproducible way) by the people involved in cold fusion experiments, can be reasonably attributed to the spontaneous and uncontrolled growing-up of fractal nanostructures on the Pd surface. In our opinion, even the Sr and Cs transmutations obtained in the experiments carried out by Iwamura et al.A at Mitsubishi Heavy Industries, Yokohama, Japan, which occur on the surface of the P d / P d - C a O / P d multilayer, could be due to the formation of fractal-like structures produced during the multilayer fabrication process. The present work deals with experiments aimed at the production of nanostructures on Pd wires both by anodic oxidation (in situ) and air oxidation (in situ and ex situ). 2. Experimental Procedures 2.1. Cells and

Electrolytes

The cell geometry and the experimental set-up were reported in detail in our previous papers.5"8Along the last year, about usual electrolytic experiments, we make two specific one in order to compare and cross check the results about new elements detected by ICP-MS, using light and heavy electrolytes. The cell and experimental set-up were almost the same as described in Refs. 5-8. We just changed the composition of cell (from chemical glass to quartz) in the last experiment with deuterium (b-type), as detailed in Ref. 8. (1) Hydrogen loading: Th(N0 3 ) 4 = 5 cm 3 (concentration 1 0 - 3 Fortuna) cell. (2) Deuterium loading: Th(N0 3 ) 4 = 6 cm 3

main solution 750 cm 3 (C 2 H 5 OH 95%, H 2 0 5%); (with 1 cm 3 = 1 mg of Th in D 2 0); Hg 2 S0 4 = 7 cm 3 M, in D 2 0) - Chemical glass (Schott Duran like, brand main solution: C 2 H 5 OD = 1005 cm 3 , D 2 0 = 89 cm3; (with 1 cm 3 = 1 mg of Th in D 2 0 ) ; Hg 2 S0 4 = 8 cm 3

379

(concentration 10~ 3 M, in D 2 0); NH 4 OD (0.16 M, in D 2 0 ) = 6 cm 3 - Ultra pure quartz cell. 2.1.1. Procedure for the anodic oxidations in situ The Pd wires were H, D loaded up the maximum of R/Ro (H,D /Pd ~ 0.75) by a current density of 5-10 mA/cm 2 . The wires were then anodically de-loaded with a current density of 1-2 mA/cm 2 and when the de-loading reaches the point R/Ro —1-1 or less, the current is raised to 5-20 mA/cm 2 and kept for a few minutes until full deloading. 28ago05a-10_17 1.8

120

1.6

E 8 1.4 Of -40 1.2 -80

-120

1 2.03 x 1 0 s

2.035 x 1 0 s

2.04 x10 5

2.045 x 1 0 s

2.05 x 1 0 s

Time (s)

Figure 1. R/Ro ratio versus time using optimized anodic oxidation and electrolyte composition. The solution is quite insulating (main liquid is vacuum-distilled andlOO nm filtered C2H5OH+H2O, few salt are dissolved): the cell voltage is 135 V even at only 30 mA with an anode-cathode distance of 4 cm.

2.1.2. Electrolytic

hydrogen loading after the anodic oxidation

in an alcohol

solution An example of very good result, using the combined effects of previous Pd anodic oxidation, proper electrolyte composition and effect of cathodic current, is shown in Fig. 1. The loading rate is extremely high and after 300 s the maximum of R/Ro is reached and surpassed. After that, the loading proceeds still at a surprisingly high rates up to values of R/Ro down to 1.2 (right-hand side of the Baranowski curve), within ~700 s, and down to 1.15 within 1500 s. It should be noticed that without the anodic oxidation the time for loading up to i?/i?o — 1.6-1.5 (right-hand side of the Baranowski curve) is measured by the tens of hours.

380

These results indicate that a proper anodic oxidation produces a very active surface. On the basis of Arata experiments, such activity could be explained as due to the formation, just at the surface of the wire, of something similar to Arata's true nano-particles (embedded in a matrix of ZrO^)2.1.3. Electrolytic deuterium loading after the anodic oxidation Generally, the loading experiments carried out with electrolyte b-type showed lower loading rates and lower maximum (final) loading with respect to the ones with electrolyte a-type. Typically the maximum loading did not exceed the one correspondent to R/Ro — 1-6 (right-hand side of the Baranowski curve). Anyway, deuterium-based electrolyte some times showed anomalous effects like excess heat and "new" elements as detected by ICP-MS (routinely) and (sometimes) SEM microanalysis. 2.1.4. ICP-MS results In consideration of the fact that all our previous electrolytic loading experiments in both (a) and (b) electrolytes, included anodic de-loading cycles, i.e., anodic oxidation, we routinely examined electrolytes, wire and sediments in order to check whether some transmutations had occurred. The main motivation of ICP-MS analysis was the results of Sr to Mo transmutation, shown in a very elegant experiment, by Yasuhiro Iwamura team (at Mitsubishi Heavy Industries, Yokohama, Japan), in 2002.4 We recall that, at that times and since 1998, we were using Sr as main electrolyte in our heavy water and/or heavy ethyl alcohol mixtures. We detected 9 some Mo in our Sr based electrolyte experiments, confirming the Iwamura results using a very different environment (liquid electrolyte instead of pure and pressurized deuterium gas). The latest results about main new elements, detected by a high resolution ICPMS, are reported in Table 1 and were presented at ICCF6. 8 See Table 1 comments for further details. 2.2. Deuterium

Self-loading

after Electrolysis

and SEM

Analysis

In many of the previous electrolytic D loading experiments, after some anodic oxidation cycles had been carried out, we found evidence (although not fully reproducible) of spontaneous deuterium self-loading, i.e. without applied electrolytic current, of the Pd wires immersed in the electrolyte. The deuterium was absorbed from the gas dissolved in the solution due to previous electrolysis. This assertion is demonstrated by the fact that the value of the loading is reversibly controlled by controlling the concentration of the dissolved D2 through alternatively bubbling Ar/D2 , as shown in Fig. 2. In Fig 2, at the time 269,500 s, the anodic stripping was ended (the current, from —9 mA was returned to 0 mA). Almost immediately, the wire started to absorb

381 Table 1. Main new elements detected in light alcohol-water (Scott Duran type) and heavy alcohol-water (quartz) cell. All the reagents Th(NOs)4 (at 1 rng/ml concentration) and Hg2S04 (10~ 3 M) are i n D 2 0 . BKG and reagents subtracted. 1 Count = about 5 X 10 1 0 atoms. In bold characters are reported value of new elements, about deuterium experiments, larger than a factor 10 in respect to hydrogen one. Element (isot. ab. %)

HJoading Exp. counts

D-loading Exp. counts

Comments

p

0 0 2.3 x 10 6 63/65 = 2.20 6.2 x 10 6 3.1 x 10 4 Normal 6.5 X 10 6 1.86 X 10 4 1.16 X 10 4 80 4.5 x 10 5 1.1 x 10 3 4.3 x 10 7

6.4 x 10 6 1.8 x 10 7 2.5 x 10 7 63/65 = 2.11 4.9 x 10 7 8.2 x 10 4 Depleted of 5% 2.6 x 10 6 1.31 x 10 5 4.42 x 10 4 900 1.38 x 10 7 1.0 x 10 4 10.8 x 10 7

BKG = 4E3 BKG = 1E6 Nat. 63/65 = 2.25

39

K

Cu Zn Rb 108 P d (26.5%) Ag 140 Ce(88.5%) W Tl Pb U 195 P t (33.8%)

Marker anode dissolution

19-20JAN05

2.68 x10 5

2.7 x105

2.72 x10 5 2.74 x10 5 Time (s)

2.76 x10 5

2.78 x10 5

Figure 2. R/Ro versus time (seconds) with the effects of D2 - ^ A r ^ D 2 intake and anodic stripping current (A). The values of R/Ro are "twin" because we introduced the procedure to measure also the Resistive Thermal Coefficient (RTC), see later.

382

the deuterium dissolved in the solution and the R/Ro increased from about 1.05 to about 1.405. At the time 273,500 s large amount of Argon gas was introduced, by bubbling it inside the solution. Immediately, the R/Ro started to decrease. At the time 275,500 s, after the R/Ro decreasing (because of argon effect) from 1.405 to 1.375, D2 gas was added again. The R/Ro value again increased, showing reversible and controllable effects. At the time 277,300 s, when the R/Ro increased to 1.45, the intake of D2 was stopped and Argon was added again. At the end, another anodic de-loading was carried out (at -6 mA) in order to fully de-load the wire. Moreover, observing Fig. 3, we would like to stress that there is unquestionable experimental evidence that the spontaneous self-loading following anodic oxidation reaches values of D/Pd over the well-known thermodynamic limit. In other words, we expected a R/RQ ratio less than 1.8 but we observed a value much larger, close to 1.95-2.0. Such value is equivalent to a deuterium pressure of about 8-10 times larger than 1 bar, i.e. the D2 pressure used in the cell (e.g. time 287,000-300,000 s). 19-20JAN05

0.002

- -0.008

2.8 x10 5 Figure 3. Fie. 2.

2.85 x10 5

R/RQ versus time. R/Ro

2.9 x10 5 Time (s)

2.95 x10 5

3x105

is about 2 instead of 1.8 expected. Other comments like

In Fig. 3, it is shown the spontaneous loading of deuterium gas dissolved in solution (time 282,000-300,000 s). At the time 279,000 s the anodic de-loading was ended in an argon atmosphere. At the end of the anodic cycle a weak selfloading was observed. Later (time 281,000 s) argon was again added for calibration purposes. At the time 282,000 s deuterium gas (at about NTP, overpressure of only 50 mbar) was finally added and self-loading started immediately. The R/RQ values are >2.0 (time 290,000 s) because of the effect of residual stress (R/Ro at D/Pd = 0 is increased to about 1.05 with respect to 1.00 at the time "0" at the beginning of the experiment). In other words, the wire was de-loaded (at the time 282,000 s) and intentionally we did not correct (by mathematic calculation)

383

the value in such experiment because we decided to "monitor" the value of the residual stress versus time. 2.2.1. SEM micro-photography and microanalysis In Figs. 4-6 are shown some pictures, by SEM microphotography, of Pd wire before (Fig. 4) and after (Figs. 5 and 6) D electrolytic loading. Elemental analysis (by microprobe) of some "white" area of Fig. 6 are shown in Fig. 7. Figures 4-7 are the same as presented at JCF6. The wire analyzed was about 10 cm long out of 60 cm total. The new elements are concentrated within about 15% of the total length, in a random like distribution.

Figure 4. SEM picture of Pd virgin wire, before electrolysis. The wire is contiguous to used one of Fig. 4.

It is clearly shown the problem coming out from anode dissolution and its deposit at Pd cathode surface. Such deleterious effect, in respect to H and D absorption in Pd, is not yet solved (despite our deep efforts). We recall that, unfortunately, the over-volt age of H and D at Pt surface is close to zero. We are convinced that one of most important reasons of poor deuterium loading into palladium, as reported from several researchers, is very often the platinum coating (from the anode) at palladium cathode surface, specially at large current density (over 500 mA/cm 2 in water solution). It is interesting to note that, apart sensitivity, the same elements are detected from both SEM and ICP-MS. In other words, the ICP-MS results are "safe" and are not instrumental fakes.

384

Figure 5. SK\! picture of a usf\l wire, heavy solution clc-tmlysis. The "new" HIMIUMIIS and P t deposit (from anode) are concentrated in few spot area (about 15% of wire length).

2.3. Air Oxidation

of Pd and

Coating

As we have shown, in our electrolytic loading experiments, we observed the phenomenon of spontaneous deuterium loading, i.e. without the application of any electrolytic current (self-loading). After several years of observations and specific

Figure 6.

Details of deposits as reported in Fig. 5.

385

tests, we realized that large self-loading occurred only at the end of certain anodic cycles, in specific electrolytes. In particular, we found that the self-loading effect obtained with water electrolytes was almost negligible (R/RQ « 1.1), while with hydro-alcoholic electrolytes, both a- and b-types, the effect was higher. By optimizing the anodic cycle it was possible to reach self-loadings up to R/RQ = 1.75 (left-hand side of the Baranowski curve) with H 2 and R/R0 = 1.95 (left-hand side of the Baranowski curve) with D2.

5000 Pt

Counts

0.000

keV

20.480

Figure 7. SEM elemental analysis of one of "white" area has shown in Fig. 5. The, unwanted, large deposition of Pt at Pd surface is clearly detected. Moreover, also Zn and Cu, detected by ICP-MS analysis, are re-confirmed.

SEM microphotography of the Pd wires, which presented strong self-loading effects, show the presence of thin porous structures on the surface of the wire. It was also observed that during the anodic cycles in hydro-alcoholic electrolytes a significant diffused pitting corrosion occurs both of Pd and Pt electrodes. ICP-MS revealed a consistent presence of Pt in the electrolyte, in the sediments and on the Pd surface. These facts suggested that in such electrolytes the anodic cycles produced strong oxidations of the Pd (useful) and Pt (deleterious, see previous discussion about over-voltage) wires. These considerations led us to try a high temperature air oxidation of Pd wires as an alternative and more practical mean for obtaining active palladium surfaces. Since the first trials we found out that this simple procedure is scarcely effective. As a matter of fact it produced slight and unstable self-loadings and only for once. We considered that during the anodic cycles, in addition to anions, negatively charged particles are electrophoretically deposited on the Pd electrode and that this effect is enhanced in an alcoholic environment, so we thought that for a significant self-loading to occur, the presence of an impurity layer, intimately adherent to the

386

oxidized surface, might be a necessary condition. So we resorted to artificially apply such impurities to the oxidized Pd wire in the form of colloidal silica. 2.3.1. Procedure for the preparation of the samples A thin (50 /xm diameter) and long (60 cm) Pd wire was Joule heated in air (=600 mA for 60 s) at about 700°C in order to get a thin layer of PdO.

01-03MAR05_KI

I a&%Stt)»»a«S&>

" Pac

|

*

1.8

-

0.8

0.6

1.6

cf? 1.4

- R/Ro_d

- 0.4

1

| 0.2

1.2

0

fe^SU^SSSUKSS*

5x10

4

1x10

5

1.5 x 1 0

s

2 x10

s

2.5 x 1 0

5

3 x10s

Time (s) Figure 8. Loading characteristic of a virgin palladium wire: loaded at room temperature with lbar of deuterium gas. In order to "activate" the Pd surface, it was made a preloading cycle (from time 0 to about 60,000 s) with D2 gas, 293 K, 1 bar and later allowed to decrease, very slowly, the deuterium content in the cell. Even neglecting the activation time, the time needed to reach the thermodynamic limit of R/Ro = 1-82 is as large as 220,000 s. Such values (i.e. R/RQ and time) are in agreement with data usually reported in the literature. As standard in our procedure from about 2 years, we cyclically inject electromigration ac current (square wave, 10 kHz) with low (about 10-15 m W ) and high power (700-800 mW) in order to calculate the Resistive Thermal Coefficient versus D / P d ratio.

After such a heat-treatment the wire was immerged into a diluted solution of colloidal silica, and then heated-^cooled^heated^cooled again several times. 2.3.2. Measurements Virgin Pd wires (no treatment) exposed to D2 gas at 1 atm and ambient temperature, usually reach a maximum loading, corresponding to an electric resistance ratio R/R0 « 1.82, in over 2 days (Fig. 8).

387

The wires, treated according to the reported procedure, exposed to hydrogen or deuterium in the same condition, instead, showed extremely fast, and quite larger, loading rates. In Fig. 9 is shown the case of a wire exhibiting an astonishingly high loading rate: the electric resistance ratio (R/RQ) of the wire exposed to a 1 atm D 2 gas, at 24° C, reached the value of 1.90 in about 100 s. The maximum R/R0 value of 1.98 (D/Pd S 0.75) was reached 2 min later, and remained stable for a long time. Further details, by the authors of this paper, are shown in the JCF6 proceedings. 19APR05.196

0.15

0.05

5.74 x 1 0 4 5.75 x 1 0 4 5.76 x 1 0 4 5.77 x 1 0 4 5.78 x 1 0 4 5.79 x 1 0 4

5.8 x 1 0 4

Time (s) Figure 9. (1 bar).

Loading ratio versus time of a Pd wire treated by oxidation and silica. D gas loading

It was also found that if during the treatment procedure of the wires, the step involving the immersion in colloidal silica is omitted, the loading rates are significantly lower and after a couple of hours R/RQ starts to decrease (de-loading). 3. Safety Rules-Procedures The following procedures have to be carefully followed to avoid explosions because possible mixing of hydrogen (and or deuterium) with oxygen and highly catalytic effect of palladium surface, activated because growing of nano-structure at its surface. We remark the safety procedures are quite easy in our experimental setup because we take fully advantage of our procedure to measure both the R/RQ value and the Resistive Thermal Coefficient (RTC) of Pd wire versus loading (see our

388

reports at, Asti5, ICCF11, and JCF6 for further details). In such a case, we used the ratio between the RTC value made by injecting alternatively low (about 15 mA equivalent to about 10 mW of power dissipated, called R/R0JL) and high (about 120 mA, equivalent to abut 700 mW power dissipated, called R/R0J1) AC current along the thin Pd wire. Because very different thermal conductibility of gas was adsorbed (H 2 , D 2 , He, Ar, Air, and "vacuum"), after proper calibration once for ever, it is very easy to understand the real composition of gas atmosphere inside the cell.

3.1. Typical

Situation

New Joule heating of the wire (0.05 mm diameter) that previously was H and D loaded. The aim is in situ new oxidation by air to get fresh PdO for further tests. The procedure is detailed, step by step, as follows. (1) Intake, and flux, Ar gas. * Measure continuously R/RQ-L and R/RQ-H. * End the large intake of Ar only when the ratio between R/RQJI and R/RO-L increases largely (and stabilize) due to the lower thermal (at 0°C, 1.013 bar) conductivity of Ar (16.36 mW/m*K) in respect of H 2 (168.35 mW/m*K) or D2(130.63 mW/m*K). (2) Increase, slowly, the DC I_electromigration (/.em), from 0 to 350 mA, keeping Ar flux at low values. (3) Observe deloading. (4) Wait for complete deloading (10-30 min, depending on wire coating). Decrease 7_em from 350 to 0 mA. (5) Check R/RQ-L value: if close to 1.0, go to step 6, otherwise wait until full deloading by injecting 7_em again at large value (350 mA). (6) Intake of He for test: the ratio of R/RQJI versus R/R0-L as to decrease largely in respect to Ar filling, due to the larger thermal conductivity of He(142.64 mW/m*K) in respect to Ar. (7) Make vacuum (e.g. oil-free membrane pump, limit about 10 mbar) to pumpout He. (8) Intake of dry air (thermal conductivity, at 0°C 1.013 bar, 23.94 mW/m*K) at STP. I.em = 0 mA. Measure R/R0-L only. (9) Increase Lem from 0 to about 600 mA. Wait 1 m at 600 mA. Observe the R/RQ instantaneous increasing due to large Lem: R/Ro about 3. At R/Ro = 3 the wire temperature is about 700°C. (10) Decrease slowly (in about 2 m) /.em from 600 to 0 mA. Repeat the cycle three times. (11) Check the R/Ro value and recalibrate the value, if necessary.

389

(a) Reintroduce the R/R0JL and R/R0JI cycles. (b) If all was correct, the values of R/RQJL and H, in air at NTP, are respectively: 1.00, 1.13 (input current of about 15 and 120 mA). (12) Make vacuum and check if the values of R/R0.L and R/RoJi have the proper values as expected. They are used the calibration data obtained at the beginning of the experiment. (13) Wash the cell with Ar or He. Later on, make vacuum again. (14) Intake of H2 or D2 and observe loading and cell temperature. By the way, we observed that some residual He gas, at the order of 1%, instead of usual Ar, has a beneficial effect about both maximum value of loading and anomalous effects generation. Such phenomena as to be more deeply investigated. (15) Stop immediately any current, and inject/wash with He or Ar, if cell temperature and/or pressure increase in an anomalous way. 4. Conclusions According to us, almost all of positive experimental results (excess heat, transmutation, and particle emissions) in cold fusion experiments (Fleischmann, Takahashi, Arata, Iwamura, Mizuno, Celani, McKubre, Swartz, Storms, Preparata-De Ninno-Del Giudice, Miley, Violante, etc.) can be rationalized as the effect of nanostructures at the Pd surface. It is very difficult to produce such nano-structures (almost all, except Arata, Iwamura, and Celani) obtained just by chance. Moreover, such nano-structures are not stable over time. We begin to develop a simple procedure to obtain nano-structures, both by electrolysis (routinely produced also during the usual cathodic regime: specific electronic circuit and procedure developed from our Group since 2004, patenting) and by addition of colloidal silica on oxidised Pd surface (since March 2005, gas loading). In some aspects, the latter method is similar to Yoshiaki Arata procedure that was the Pioneer about nano-particles production for cold fusion studies. The kind of colloidal silica (5-10 nm dimension, low Na content), that up to now gives the best results, was specially developed (after 5 years of efforts), by an Italian chemical company, according to our request. We think that the nano-structure interpretation of anomalous effect in deuterated metals will bring soon to some technological device: boiler using liquid electrolyte, even some turbine engine using pressurised high temperature gas loading method. More systematic work is necessary in order to elucidate all the possibilities that come because nano-size materials (specially pure Pd and/or Pd-based alloys) properly coated/embedded by a third element. Finally, as shortly shown also during ICCF12, we get indications that some anomalous heat seems coming out, from a new pressurised (4 bar) cell (SS), using even the hydrogen gas when the temperature of the wire, heavy coated by colloidal silica, was forced to reach about 200°C (by Joule heating).

390 Acknowledgements We are really indebted to Prof. Akito Takahashi (Osaka University, J a p a n ) , Prof. Yoshiaki A r a t a (Osaka University) and Dr. Yasuhiro Iwamura (Mitsubishi Heavy Industries, J a p a n ) , because stimulating discussions, critics and suggestions about the role of nanostructures in Condensed Matter Nuclear Science experiments. We cannot forget t h a t the pioneer work of Prof. A r a t a about nano-particles (starting with the use of "palladium black" at different grain sizes) which opened our eyes about new interpretation of some of our old d a t a t h a t never get satisfactory explanation. Other general and long discussions with Prof. H. Y a m a d a and S. Narita (both at Iwate University, J a p a n ) , Prof. A. K i t a m u r a (Kobe University, J a p a n ) , Prof. T. Mizuno (Okkaido University, J a p a n ) , Prof. S.E. Jones (BYU, Utah, USA), Dr. E. Storms (Lattice Energy LLC, New Mexico, USA) helped us to elucidate the very complex behaviour of P d surface during and after, very different, electrolysis operating conditions. Dr. W . Collis (Heidi Limited, 14055 Boglietto di Costigliole, Italy) helped us during the very long a n d tedious analysis of possible elements coming out by ICP-MS instrument. T h e special software program (ENSAT) he developed, about possible "transmutation" channels, was really useful to speed-up the analysis. References 1. Y. Arata, The formation of 'solid deuterium' solidified inside crystal lattice and intense solid-state nuclear fusion (cold fusion), II Nuovo Saggiatore (Bollettino SIF, ISSN 1827-6148), Vol. 20, No. 5-6, pp. 66-71 (2004). Also at: http://www2.sif.it/riviste/nsag/nsag-2004-05-06/07.pdf; ** Y. Arata and Y. Chang, Proc. of ICCF10, 24-29 August 2003, Cambridge, USA (Edited by P. Hagelstein and S. Chubb), World Scientific (ISBN 981-256-564-7) pp. 139-157 also at http://www.lenrcanr.org; *** Private Communications. 2. A. Takahashi, Proc. of ICCF10, 24-29 August 2003, Cambridge , USA (Edited by P. Hagelstein and S. Chubb), World Scientific (ISBN 981-256-564-7), pp. 447-454, 809818 also at http://www.lenr-canr.org; ** Conf. Proc. (Edited by H. Yamada) of JCF4, JCF5, JCF6 also at http://wwwcf.elc.iwate-u.ac.jp/jcf/;*** Private Communications 3. F. Celani, A. Spallone et al. Study of deuterium charging behavior in palladium and palladium alloy plates, changing surface treatments, by [is pulsed electrolysis, Proc. of ICCF5, Montecarlo, Monaco, 9-13 April 1995, pp. 411-418. 4. Y. Iwamura et al, Jpn. J. Appl. Phys. (2002) 4642; ** Y. Iwamura et al, Proc. of ICCF10, 24-29 August 2003, Cambridge. USA (Edited by P. Hagelstein and S. Chubb) World Scientific (ISBN 981-256-564-7) pp. 435-446; *** Proc. of IGCF11, Marseilles, France, 01-05 November 2004 (Edited by J. P. Biberian), World Scientific (ISBN 981256-640-6) pp. 339-350, also at http://www.lenr-canr.org; **** Conf. Proc. (Edited by H. Yamada) of JCF4, JCF5 also at http://wwwcf.elc.iwate-u.ac.jp/jcf/ 5. F. Celani, A Spallone et al. Proc. of ICCF10, 24-29 August 2003, Cambridge, USA (Edited by P. Hagelstein and S. Chubb) World Scientific (ISBN 981-256-564-7), pp. 379-397 also at: http://www.lenr-canr.org 6. F. Celani et al, Further tests on composition and isotopic anomalies when Pd thin cathodes are electrolized in acidic C2H5OD/D2O mixture added with Th-Hg salts at micromolar concentration, Proc. of the 5 Meeting of Japan CF Research Society,

391 15-16 December 2003, Kobe University, Japan. (Edited by H. Yamada), pp. 41-45, also at http://wwwcf.elc.iwate-u.ac.jp/jcf/ 7. F. Celani et al., Innovative procedure to measure, in situ, resistive thermal coefficient of H(D)/Pd during electrolysis and cross-comparison of new elements detected in T h - H g Pd-D(H) electrolysis cells, Proc. of the ICCF11, Marseilles, France, 01-05 November 2004 (Edited by J. P. Biberian), World Scientific (ISBN 981-256-640-6), pp. 108-127, also at: http://www.lenr-canr.org 8. F. Celani et al, Further studies, about new elements production, by electrolysis of cathodic Pd thin-long wires, in alcohol-water solutions (H,D) and Th-Hg salts. New procedures to produce Pd nano-structures, Proc. of the 6 Meeting of Japan CF Research Society, April 27—28 December 2005, Tokyo, TIT, Japan (Edited by H. Yamada) also at h t t p : / / wwwcf.elc.iwate-u.ac.jp/jcf/ 9. F. Celani, A. Spallone et al. Proc. of the 4 Meeting of Japan CF Research Society, 17-18 October 2002, Japan (Edited by H. Yamada), pp. 17-21, also at http://wwwcf.elc.iwate-u.ac.jp/jcf/

USING RESISTIVITY TO M E A S U R E H / P d A N D D / P d LOADING: M E T H O D A N D SIGNIFICANCE

M . C . H . M C K U B R E A N D F.L. T A N Z E L L A SRI International,

Materials

Research Laboratory, 333 Ravenswood CA 94025, USA E-mail:[email protected]

Avenue,

Menlo

Park,

The resistance ratio method is the most frequent technique used to determine the extent of interstitial loading of hydrogen or deuterium atoms into palladium electrodes, or extended structures used in electrolytic or gas phase cold fusion experiments. Specifically, advantage is taken of an empirical relationship between the measured resistance, R, normalized to that of the same body at the same temperature in the absence of hydrogen isotope, Rg, hence R/Ro, and the atomic fraction occupancy of octahedral interstitials, x = H / P d or D / P d . This method was first suggested and employed in cold fusion studies by the present authors, and received immediate and widespread acceptance because of the ease with which this experimental technique could be used to make in situ, real-time measurements of a parameter, D/Pd, anticipated or hypothesized at that time to relate to cold fusion heat excess or nuclear production. We take up this topic again 15 years later in an attempt to clear up some errors and misunderstandings regarding the resistance ratio method and its application in cold fusion studies. The relationship between R/Ro and x is empirical. That is, calibrations are only as good as the experiments that support the shape of the curve and cannot be used outside the range (P, T, x) in which data are taken. The original calibration (unaccountably and erroneously immortalized as the "famous Baranowski curve") involved an extrapolation of known data into the region of cold fusion interest in the D - P d system, at x > 0.6. Present theory and results focus new attention on the very high loading region as x approaches or even exceeds unity, where double occupation of octahedral sites, tetrahedral site occupancy, new phase formation or new electrical states, may be relevant to the underlying physical process of excess heat and nuclear production. Rather than simply using the resistance ratio as a qualitative tool to determine whether an electrode is better or lesser loaded, it is now important to obtain accurate quantitative information for x close to unity. With further experimentation and analysis of published data it is apparent that the curve originally published in 1990 is in error in the high loading condition. This paper describes how this empirical fit has been improved over the years for both H / P d and D / P d by employing new data, new analysis of old data, new experimental methods and results.

1. Introduction The first paper drawing attention to resistance ratio measurement as a means to quantify deuterium loading in Fleischmann-Pons electrolytic cold fusion experiments was presented by the present authors at the First Annual Cold Fusion 392

393

Conference held in Salt Lake City in March 1990, and published in the ensuing proceeding.1'* The authors of that paper made three introductory comments: 1. None of the "cold fusion" electrolysis experiments described to data contain any means of determining the D/Pd content in situ. Yet this ratio may be a crucial difference between those experiments that have produced a Fleischmann-Pons effect and those that have not. 2. The resistance of Pd metal is a function of its hydrogen content and is in principle, the easiest way of determining the state of the Pd electrode as the experiment proceeds. 7 3. The relationship between the resistance and the D/Pd ratio is known only up to 0.65. Comparison can be made with the H/Pd system which is calibrated in resistance up to H/Pd = l.l. 8 The first two comments proved to be prophetic. A clear distinction can be made on the basis of average D/Pd loading measured by resistance ratio between successful and unsuccessful excess heat production in electrolytic Fleischmann-Pons experiments. Resistance ratio measurements quickly became and remain the most widely used method of determining loading in situ. Here we expand point 3. 2. Experimental In 1990 the resistance versus composition function had been characterized for the light hydrogen system up to H/Pd = l.l. 8 This function was less well specified for D/Pd. Our initial attempt to estimate the curve based on known data 9 up to D/Pd = 0.65 combined with the assertion that the resistance ratio maxima would occur at the same composition of H and D, resulted in the somewhat distorted curve presented at ACCFl 1 and replotted here as Fig. 1. The fourth-order polynomial extrapolation plotted as a grey line in Fig. 1 formed the basis of all early estimates of D/Pd loading from resistance ratio measurements. Between 1990 and 1993 a campaign of measurements was undertaken to refine the calibration of the resistance curve for D/Pd. A number of methods were used to measure composition independent of resistance in the D/Pd system, each with important advantages and disadvantages. Some of these methods are briefly reviewed here: I. Macro-gravimetric. The most direct method to determine the extent of absorbed hydrogen isotope is to weigh the cathode after prolonged loading. Both the resistance and mass measurement can be performed ex situ after washing and drying the electrode. The primary disadvantages being relatively low accuracy because of systematic errors due to the presence of surface adsorbed non-hydrogen species and absorbed but non-interstitial hydrogen, and the lack of access to the high loading region because of rapid deloading. *Although the atomic ratio D / P d had been anticipated 2 and hypothesized 3 - 8 at that time to relate to cold fusion heat excess or nuclear production.

Micro-gravimetric. An in situ gravimetric measurement was reported by NRL also at ACCF1. 2 Cheek and O'Grady used a quartz crystal microbalance to measure the mass of a deposited palladium surface film operated as a cathode. A critical difficulty with this method is the lack of access to the high loading region due to buoyancy effects associated with the presence of internal D 2 filled voids and surface attached D 2 bubbles at current densities sufficient to produce high loading. This method is also affected by roughening and spallation of the Pd film from the quartz support at high loading and has seldom been used. Dilatometry. A number of people but notably Storms 10 took advantage of the lattice expansion that occurs when hydrogen isotopes occupy the octahedral interstitial sites in the fee Pd lattice. Either linear extension or volumetric expansion measurements can be used to estimate the extent of hydrogen isotope absorption provided this is wholly interstitial. A very important outcome of the extensive work by Storms using the technique was that a significant fraction of the hydrogen or deuterium atoms absorbed by palladium recombine in closed voids within the metal causing compressive stress and volume expansion greater than that attributable to the change in lattice parameter. Storms called this parameter "free volume". Electrodes with a large fraction of free volume tend to load poorly and to not produce excess heat. 10 Oxygen displacement in closed cells. The equations that govern the cathodic absorption of H (or D) in thermodynamically closed cells can be written for 2.1 2.0

•?

f

H D

1.9

\

\

/

1.8 1.7

CD

' '%

V

1.6

\ \

V_ \

CD

o 1.5 c CO 1.4 *—> c/j CO 1.3 CD

\

cr 1.2 1.1 1.0

i.

V ! --

0.1 0.2

-r -

r - 1 U .. rn J • i i I ill 111 LiH * "' - _ . 0.3' '"0.4 0.5 0.6 0.7 0.8 0.9 1.0 ^

Mole fraction (H,D)/Pd Figure 1.

Original calibration curves. 1

1.1

395

basic light water electrolytes as: Cathode: H 2 0 + e~ => OH" + H a d s Cathode recombination: Hacis + H a( j s =>• H2 Cathode absorption: Hads =4> H a b s Anode: 2 0 H " => H 2 0 + 2e~ + O a d s

(1) (2a) (2b) (3)

Anode recombination: O a a s + Oads => 0 2

(4)

Molecular recombination: 2H2 + 0 2 => 2H 2 0

(5)

In the absence of reaction (2b) the rates of production and recombination of H2 and 0 2 are stoichiometrically balanced. Hydrogen occluded in the cathode by reaction (2b) is not available to recombine to water on the catalyst surface (5), resulting in a net production of 0 2 gas. This gas can be measured as a pressure increase (at constant volume, V, and temperature, T) or a volume increase (at constant pressure, P, and T). One favored method is simply to displace an inert liquid onto a balance to be weighed. In the presence of an ideally performing catalyst this method is easily employed and relatively reliable. As is true for most of the methods discussed here, it is not capable of distinguishing between interstitial absorption and hydrogen occluded in free volumes within the Pd bulk. This method was widely used by Riley et al., at the National Cold Fusion Institute (NCFI). 11 The data obtained from their studies were used to refine the SRI resistance ratio versus loading curve. V. Hydrogen displacement in closed cells. In general recombination catalysts operate more reliably at gas concentration ratios well away from the stoichiometry point (2:1 H 2 :0 2 ). Method IV also has the disadvantage of making the environing and dissolved gas concentrations oxygen rich, thus lowering the H2 (or D 2 ) partial pressure and reducing the maximum loading. A method was developed at SRI 12 to precharge sealed and thermodynamically closed electrolytic cells with a controlled atmosphere of hydrogen gas. In this situation the net loading that results from Eq. (2b) reduces the moles of H 2 (or D 2 ) in the gas phase. This can be readily measured as a pressure change (at constant T and V) or volume change (at constant T and P). VI. Stripping coulometry. An anodic reaction process involving successively the reverse of reactions (2b) and (1) can be used very accurately to titrate loaded H (or D) from the lattice provided that the surface atom recombination reaction (2a) is avoided. This reaction can be effectively poisoned by electrodepositing heavy metals on the cathode surface. Since this also prevents absorption the co-deposition of metals such as Hg is best done at or near the end of hydrogen loading. A procedure of this type was developed for H and D loading of long thin Pd wires by Celani's group at INFN Frascati. 13 This method was further developed collaboratively by Tripodi at SRI for the purpose of measuring temperature effects on resistance. 14

396

VII. X-ray diffraction. The position of Pd atoms in their sublattice of PdH x or PdDz is a function of the loading, x. Although reasonably well established for PdHa;, particularly for x < 0.85, no reliable information exists for the condition of interest in cold fusion experiments, PdDx for x > 0.85. A collaboration between the groups at the US Naval Research Laboratory (NRL) and ENEA, Frascati in Italy has been established to redress this deficiency.15 As well as the expected increase in lattice parameter with increasing octahedral occupation, the researchers are also interested in pursuing evidence for tetrahedral site occupation, double occupation of octahedral site or new phase formation. VIII. Neutron diffraction: Cold fusion experimenters and theorists are more interested in the positions occupied by deuterons in the PdD x sublattice, as x approaches or exceeds unity, rather than in the relative positions of Pd atoms. In principle this information can be accessed directly in neutron scattering experiments. It is possible than no single experiment is of greater importance to the cold fusion community in the high-loading, heat-producing condition of PdDa;^ x . An attempt to perform an in situ electrolytic loading experiment in collaboration between SRI and Los Alamos National Laboratory, LANL, was unsuccessful for technical reasons in 1994 but further attempts should be considered. As the result of a large number of experiments to correlate loading and resistance ratio at SRI 12 and elsewhere11 made mostly using methods I, IV and V, the curve originally constructed in 1990 and shown as Fig. 1 was refined in 1993. Two versions of this curve were published; 12-14 these are replotted here as Figs. 2 and 3. Figure 3 also took advantage of data originally published by Baranowski et al., in 1990,19 but comprehensively re-analyzed at SRI in 1993. These data were also included in the SRI curve (Fig. 4) that sought to distinguish between successful heat producing cells (labeled in red) and unsuccessful heat producers (green) on the basis of the maximum loading or minimum resistance attained on the right-hand side of the resistance maximum. This curve provided important confirmation of the need to measure loading and the utility of the resistance ratio method. Absent a complete set of calibration data covering the entire range of D-Pd composition the curves in Figs. 2 and 3 were constructed according to the following rules: 1. Linear multiple relationship between the H and D loading curves. 2. The resistance ratio maxima for H and D occur at the same atom fraction. 3. The high loading data for D-Pd conform with minimum standard deviation to the 1990 data of Baranowski et al.19 A comprehensive review of the literature was undertaken to estimate better the position of the H-Pd resistance-loading curve and the results published as in Ref. 20. In addition a more extensive analysis was made of the Baranowski data for D-Pd published in Ref. 19. Based on these analyses and applying rules 1-3 listed above,

397

we have constructed new curves for H-Pd and D-Pd in the high loading region. These curves are presented in Fig. 5. Also plotted in Fig. 5 are the equilibrium gas pressures needed to achieve the specified atomic ratios. The square points in Fig. 5 taken from the Baranowski data 19 exhibit an interesting kink or second order transition at D/Pd > 1.02. The origin of this feature is not known although it appears not to be present for H in the same region of composition. Another attempt to specify the resistance/loading functions for palladium made by Zhang et al.21 resulted in the curves replotted in Fig. 6. While the difference between the Zhang and SRI curves is subtle we believe that Zhang's curves fall outside the uncertainty in the literature data for H 20 and the precision of the Baranowski data for D. 19 It is also notable, although not diagnostic, that Zhang's curves for H and D exhibit maxima at different atomic ratios (cf. rule "2"above). A test of accuracy of the H-Pd curve was made directly by Tripodi and the present authors. 22 The coulometric stripping method described in method V above was used to directly correlate resistance and loading of two sections of fine Pd wire cathodes (diameter 50 ^m, length 10 cm) loaded to H/Pd « 0.98, sealed by co-

0.00

Figure 2.

0.20

0.40 0.60 H(D)/Pd

0.80

Second calibration 1993, Version 1.

1.00

398

deposition of Hg 12,13 and then stripped at very small anodic current density. The results shown in Fig. 7 do not provide a strong basis to distinguish between the Zhang and SRI curves. The knee at H/Pd ~0.57 is interesting and appears to be a real feature. Because of this knee, Zhang's attempt to accommodate data at loading H/Pd < 0.6 (not attempted by SRI) appears to have moved their predicted resistance maximum to lower loading and higher maximum value. 3. Discussion The various attempts to characterize the position of the resistance versus loading curves for H-Pd and D-Pd can be summarized in terms of a few critical constants: 1. The maximum resistance value of the resistance ratio, -R/_Romax2. The value of the atomic ratio at the point of maximum resistance, x m a x 3. The value of the resistance ratio at a loading x = 1, R/Ro x=\. Table 1 shows how values of these constants have changed in 16 years of experimentation and analysis.

RIR

°

1 +3x-15.13x 2 +44.16x 3 -49.12x 4 +17.58x 5

0.00 0.10 0.20 0.300.400.50 0.600.700.80 0.901.00 H (D)/Pd Atomic ratio Figure 3.

Improved calibration 1993.

399

FURo T1-2.0HFI-3

2

Figure 4. Showing the correlation between maximum loading measured by resistance ratio and successful (red) and unsuccessful (green) heat production in Fleischmann-Pons electrolysis experiments performed at SRI.

Some changes have occurred in the curve for H-Pd; a small increase in the resistance maximum and a significant increase in the position of the maximum for the SRI curve but not for Zhang's. Of far more significance to cold fusion workers

R/flO (PdB*>fl/f?o (PdB*> R/R0 (PdH^ PH2 (atrffc)-PD2 (atm.) T 40000

0.7

0.75

0.8

0.85 0.9 0.95 Atomic ratio

1.05

Figure 5. Improved calibration curves based on new data, reanalysis of H-Pd literature 2 0 and Baranowski data for D-Pd (square points 1 9 ).

400 -*--R:R, iP&Hx) —Zhang & Zhang H —Stnp Upper —Strip Lower

1

o.2o

0.30

0.40

0.50

0.60

0.70

0.80

0.90

1.00

Atomic ratio Figure 6.

SRI 2 0 and Zhang et al.21 curves and Tripodi et al.22 stripping data.

the value of the resistance at H/Pd = 1, R/RQ X=I, has dropped from ~1.35 to 1.067 for the SRI curve and below unity to 0.926 for Zhang's curve. Turning attention to the D-Pd system the expected value of maximum resistance has changed very little with reanalysis. The position of maximum resistance in D Pd has increased following that of H-Pd for the SRI curve using rule 2. The increase in this parameter for Zhang's curve is even larger. Of much greater significance in cold fusion studies the expected resistance at D/Pd = 1 has dropped from 1.5 in 1990-1994 to 1.43 in 1996 to 1.245 in the SRI curve circa 1998. The value for Zhang calibration published in 2002 is even lower at 1.222. The combined effect of moving the position of the resistance maximum to higher loading, and the expected resistance at D/Pd = 1 to lower resistance value results in a much steeper calibration curve on the right-hand side of the resistance maximum. As a consequence, when comparing the old calibration to the new, resistance ratio values interpreted as loadings in the region of interest for Fleischmann-Pons effect studies (D/Pd > 0.85) have consistently overestimated the interstitial deuterium Table 1.

Changes in loading parameters

1990

1994

H/Pd fi/fio™ xmax R/Ro x=i

Ref. 1 1.79 0.725 1-34

Refs.16-18 1.78 0.729 1.36

D/Pd R/BomaI xmax R/Ra x=1

2.00 0.725 1.50

2.00 0.724 1.50

1996

Ref. 19 2.00 0.724 1.43

1998

2002

Refs. 20,22 1.809 0.760 1.067

Ref. 21 1.820 0.732 0.926

This paper 1.96 0.760 1.245

2.01 0.772 1.222

401

content of the palladium. This systematic error is not large, but it may have important physical significance. Table 2 recalculates the maximum loading based on the minimum resistance ratio measured on the right-hand side of the resistance maximum for five historic heat producing cells operated at SRI. 12 What had previously been interpreted as maximum average loadings at or above unity when evaluated with the new SRI calibration curve result in loadings D/Pd approaching unity. Only P l a indicates a D / P d m a x > 1. This cell was operated at 4°C where the calibration curve is likely to be different. In any case, the calculated loading maximum is not outside the estimated 1% uncertainty. Thus, in experiments conducted at SRI, we have no evidence that palladium cathodes can be loaded by electrolysis to atomic ratios greater than unity. At this point it is worth discussing what is the relevance of a resistance ratio measurement of deuterium loading. The evidence is overwhelming that deuterium does not load homogeneously into polycrystalline palladium. Observations made of Pd cathode surfaces reveal that different crystalline facets load and expand at different rates, and the grain boundaries absorb (and release) D at very different rates from the bulk. Electronic transitions observed at low temperatures in highly loaded thin wires clearly indicate the presence of small zones of very differently (presumably higher) loaded material. 14 Hot spots observed either in situ with thermal imaging or retrospectively by autoradiography, 1 and local melting or isotopic effects, all suggest that the Fleischmann-Pons effect, whatever its cause, occurs heterogeneously throughout the bulk or on the surface. Indeed, since deuterium flux appears with equal footing to loading in quantifying excess heat power,23 the existence of heterogeneity (or time variability) in surface chemical potential appears to be crucial in producing excess heat in electrolytic D-Pd experiments. Given these observations and the occasional solid report of excess heat at low loading one might question the deterministic power of four terminal macroresistance ratio measurements that necessarily access a volume averaged electrode property. What might be important is simply that this property is monotonically related to the chemical potential of deuterium in the sample. The various mechanisms involved in attempts to explain the Fleischmann-Pons heat effect, the existence of a new phase or band structure, atom or ion pairing, lattice deformation to produce occupiable host sites, all depend critically on the chemical potential of absorbed Table 2.

Corrected maximum loading values.

Cell

R/R0

Pla P17 P22 P19 P12

1.20 1.27 1.30 1.45 1.55

min

D / P d old

D / P d adjusted

1.06 1.04 1.03 0.99 0.97

1.01 1.00 0.99 0.96 0.94

402

deuterium. Furthermore, the very high permeability of palladium by deuterium ensures that adjacent regions of differing chemical potential will have only transient existence or will be associated with high deuterium fluxes, a known beneficial condition. It is therefore suggested that the important lattice characteristic measured by the resistance ration is deuterium activity, not loading, in the metal. Because of the very high diffusivity of D in Pd the average D activity very closely reflects the activity everywhere in the cathode and on it's surface. We therefore expect the bulk, average resistance ratio to be reflected in excess heat rates even if the site of heat generating activity is a special environment of, on or at the surface. 4. Conclusions and Recommendations The calibration of the resistance ratio versus loading curve for deuterium in palladium originally published in 1990 and refined between 1992 and 1996 is in error. A re-evaluation of this curve based on literature and new experimental data indicates that the D/Pd loading estimates in the region of interest for electrolytic Fleischmann-Pons experiments should be revised downward. With this downward revision, it is possible that electrolytic experiments performed at ambient temperature and pressure have not achieved volume averaged D/Pd electrolytic loadings greater than unity, even in successful heat producing experiments. In order to compare loadings obtained in different experimental setups or different laboratories, it is preferable to report data as resistance ratio values, R/Ro, on the right-hand side of the resistance maximum. In this way consideration of the shape of the resistance-loading calibration curve is avoided and any improvements in this function can be easily accommodated. The issue of temperature of measurement significantly complicates the simple interpretation of a resistance ratio as an average loading, particularly in the region of interest to those studying the Fleischmann-Pons effect. The calibration curves discussed extensively here apply strictly only when R and RQ both are measured at 298 K. The temperature coefficient of resistance is known as a function of loading, and a simple mathematical correction is often made. However, this coefficient is a strong function of composition 14 and is largely unknown for PdD-j as x approaches and exceeds unity. Thus it is difficult to apply the needed temperature corrections accurately. For this reason it would be helpful for future workers to express clearly what, if any, temperature corrections have been made to R and RQ, and state the temperatures for which both values were measured. References 1. M. McKubre et al., Calorimetry and electrochemistry of the D-Pd system, in Proc. First Annual Cold Fusion Conference, Salt Lake City, F. Will, Ed. (1990). 2. G. Cheek and W. O'Grady, Quartz crystal microbalance study of Pd/H interactions, ibid. 3. G. Preparata, Theoretical ideas on cold fusion, ibid. 4. P. Hagelstein, Status of coherent fusion theory, ibid.

403

5. S. Chubb and T. Chubb, Quantum mechanics of 'cold' and 'not-so-cold' fusion, ibid. 6. J. Schwinger, Nuclear energy in an atomic lattice, ibid. 7. D. Macdonald, M. McKubre, A. Scott, and P. Wentrcek, Continuous in situ method for the measurement of dissolved hydrogen, I&EC Fundamentals 20, 290 (1981). 8. B. Baranowski and R. Wisniewski, Phys., Stat. Sol. p. 539 (1969). 9. F. A. Lewis, The Palladium-Hydrogen System (Academic Press, New York, 1967). 10. E. Storms, Fusion Technol. 29, 261 (1996). 11. A. M. Riley et al., Measurement of absorption of deuterium in palladium during electrolysis of heavy water, NCFI Final Report II, 2-123 (1991). 12. McKubre et al, EPRI TR-104195 (1993). 13. A. Spallone, F. Celani, P. Marini, and V. Di Stefano, New electrolytic procedure for the obtainment of very high H/Pd loading ratios, Proc. ICCF8 (1990), p. 191. 14. P. Tripodi, M. McKubre, and F. Tanzella, Temperature coefficient of resistivity at composition approaching PdH, Phys. Lett. A (2000). 15. G. Hubler and V. Violante, Personal communication (2005). 16. McKubre et al., Loading, calorimetric and nuclear investigations of the D-Pd system, Proc. ICCF4 (1993), p. 5-1. 17. McKubre et al., Isothermal flow calorimetric investigations of the D/Pd and h/pd systems, J. Electroanal. Chem. 368, 55 (1994). 18. McKubre et al., Chemical and metallurgical issues in the loading of D into Pd, Proc. International Symposium on Cold Fusion and Advanced Energy Sources, Minsk (1994). 19. B. Baranowski, S. Filipek, M. Szustakowski, J. Farny, and W. Wornya, J. Less Common Met. 158, 347 (1990). 20. S. Crouch-Baker, M. McKubre, and F. Tanzella, Variation of resistance with composition on the /3-phase of the H-Pd system at 298 K, Z. Fur Phys. Chemie. 204, 247 (1998). 21. W.-S. Zhang, Z-F Zhang, and Z-L Zhang, J. Electroanal. Chem. 528, 1 (2002); 571, 81 (2004). 22. P. Tripodi, F. Tanzella, and M. McKubre, Unpublished results (1999). 23. McKubre et al, Concerning reproducibility of excess power, Proc. ICCF5 (1995), p. 17.

M E A S U R E M E N T S OF T H E T E M P E R A T U R E COEFFICIENT OF ELECTRIC RESISTIVITY OF H Y D R O G E N O V E R L O A D E D Pd*

ANTONIO SPALLONE AND FRANCESCO CELANI INFN-LNF,

Via Enrico Fermi, 00044 Frascati (Rome), Italy E-mail: [email protected]

PAOLO MARINI AND VITTORIO DI STEFANO EURESYS,

Via hero 30, 00129 Rome, Italy

As reported in previous papers, we performed many electrolytic loading tests using thin P d wires, achieving loading ratios of H / P d > 0.95 ( H / P d over-loading). In particular, we defined a reproducible "loading protocol" suitable for achieving such an over-loading level, based on the use of very diluted acid electrolytic solutions (with additions of tenths of micro-moles of Ca or Sr or Li cations and some hundred nano-moles of Hg ions) and operating with electrolytic current cycles from a few mA up to one hundred mA. By observing the d a y / n i g h t cyclic fluctuations of electrical resistance, as a function of the corresponding t e m p e r a t u r e variations, of stable, long term, H / P d loadings we were able to calculate the t e m p e r a t u r e coefficient of resistivity (Kg) of the P d - H system at very high H / P d loadings. Many years ago (in 1998), we reported an unexpected value showing t h a t the Kg parameter values increase when H / P d exceeds 0.75 (i.e. after t h a t R/RQ goes beyond the 1.8 peak value, i.e. to the right side of the R/Ro/K/Pd curve). This fact was confirmed by the ISR-Stanford Group (McKubre and Tripodi) and Pirelli-Research Group (Gamberale and Garbelli). In this paper we show several measurements of Kg at different overloading values of H / P d u p to = 1 (corresponding at R/RQ = 1.12) where Kg=(13 ± 1 ) x 10~ 3 K""1, i.e. more t h a n six times higher t h a n the minimum value achieved at the R/RQ = 1.8 peak value. This result can corroborate the hypothesis t h a t a new P d - H phase (full /3-phase or the beginning of j3 + 7 phase) could occur after the H / P d = 0.75 loading ratio (at the end of a + (5 phase), as claimed by many authors as the necessary condition for excess (anomalous) heat from P d - D system (at D / P d > 1).

*This work is supported by INFN-LNF, Frascati, Italy. 404

405

1. Historical Background 1.1. H/Pd

Loading

Measurements

It is common opinion that to observe heat in excess from Pd-D system it is necessary to obtain very high values (>0.95) of D/Pd atomic ratio. 1 _ 3 Starting from 1998 we decided to perform systematic tests in order to achieve very high H/Pd loading ratio using very diluted electrolytes and thin (50 or 100 /im in diameter) Pd wires as cathodes. 4 Different electrolytic solutions have been tested by adding to the acid solution very low amounts of Ca, Sr, Li and Hg ions. In this way high H/Pd loading ratios have been achieved with a satisfactory grade of reproducibility. Several loading procedures have been performed in a wide range of electrolysis current (from a few mA up to one hundred mA) and at different Hg ion concentrations. The obtained results allowed for the definition of a loading protocol capable to insure very high H/Pd over-loading. Stable R/RQ < 1.2 values (corresponding to H/Pd ratios >0.97) can be currently achieved with an extremely low electrolytic power supply (10 V; 5 mA). 5 This procedure is based on the increase of the cathodic over-voltage (which is known to be the main controlling parameter of the H(D)-Pd loading) obtained by modifying the nature of the cathodic surface (i.e. by inducing the formation of a very thin layer of an alkaline-earth carbonate on its surface).

1.2. Temperature

Coefficient

of Resistance

Trend

The temperature coefficient of electric resistivity (Kg) of a Pd-H sample is a wellknown curve in the literature (Kg is known to decrease from 4.1 to 1.8 m K - 1 with H/Pd increase from 0 to 0.7). 6 ' 7 During 1998, after the achievement of a very high and stable H/Pd loading (=0.95), we performed a preliminary measurement of Kg resulting in a value of (3.2 ± 0.2) x 10~ 3 K" 1 within a temperature range from 77 K up to 373 K. For the first time in the literature this value showed that at values of H/Pd higher than 0.7, Kg increases.8'9 Further, this fact was confirmed by the ISR-Stanford Group 10 and Pirelli-Research Group. 11

2. Temperature Coefficient Measure 2.1. Experimental

Setup

In an electrolytic cell (solution of one liter of H 2 0 + HC1 at 10~ 4 mol) the electrodes have been located in the form of two parallel wires, of length 25 and 6.5 cm apart from each other (the Pd cathode of diameter 50 /im, the Pt anode of diameter 0.5 mm); tenths of micro-moles of Sr and hundreds of nano-moles of Hg have been added to the solution. A junction for a pick up of the voltage divided the Pd cathode in two equal segments (named: "up" and "down").

406

2.2. Experimental

Data and Fit

After applying the procedure to reach H/Pd overloading (OFF/ON current cycles, as shown in Fig. 1), if the loaded sample is found stable, we proceed with the recording of the R/Ro variations following the day/night cyclic temperature variations. The measurement campaign may last for several day/night cycles. To complete the test, Pd-H wire is de-loaded either by using anodic current or by simply turning the current off for many hours (as reported in Fig. 1) and observing the phase transition at R/R0= 1.7 (H/Pd = 0.6).

1.8 1.6 1.4 1.2

1

Time (s) Figure 1.

R/Ro

3

data are meanly stable for a enough long time (from 30,000 to 90,000 s range

Generally, as in the latter case, it is possible to check the R/Ro curve tracing back to the peak value (R/Ro = 1-78, H/Pd = 0.75) and returning to the initial value of R/Ro = 1. By considering the data in the range where the loading is stable, it is possible to record the dependence of the wire resistance on the wire temperature (homogenous with the cell temperature) and once the linearity of these data is confirmed (Fig. 2), we can make a fit to calculate the Kg coefficient according the relation (A.l) reported in the Appendix. To be considered valid to our purpose, resistance data have to be repetitive after each temperature cycle. In Fig. 1, it is reported that the load/deload procedure (V-I ON/OFF) up to R/RQ = 1.1 and R/Ro fluctuation with temperature cycles ("measure"); evidence of the /3-transition occurs during the de-loading procedure.

407

1.18 y=08tU)0ni13AP-0PS4

1.17

- I ' «,=-!?. 8x 10 *t C )

1.16 r, 1.15

^

1.14 1.13 1.12 1.11 20

Figure 2.

2.3.

21 22 23 24 25 Temperature-cell (°C)

26

Partial data of a full temperature cycle (40,000-60,000 s) well fitted by a simple line.

Results

Out of several hundred tests, only a few tens have shown a loading stability suitable for the calculation of the Kg parameter. We report in Table 1 some values corresponding to different values of Pd loading. In this table, measured values of R/Ro are reported for each of the two wire sectors "up" and "down" (generally showing similar loading values); tests ranged along a period of a year during which different wires, electrolytes and procedures were used. Table 1. Values of Kg as resulting from several tests performed at stable loading conditions and ratios (ref. room temperature at 20°C). H/Pd R/Ro ± 0 . 1 0.00 0.85 0.88-0.90 0.91 0.92-0.93 0.96-0.98 0.97-0.98 0.99-0.995

Down

Up

1.0 1.75 1.58 1.52 1.44 1.19 1.18 1.10

Kg

1

(mK- )

4.1 ± 2.8 ± 7.2 ± Ri7± S8.3 ± 9.9 ± 10.7 ± =13 ±

0.1 0.3 1 1.5 1 0.5 0.5 1.5

R/Ro ± 0 . 1 1.0 1.75 1.61 1.52 1.46 1.24 1.21 1.13

KgimK-1) 4.1 ± 0 . 1 a 2.6 ± 0.3 b 6.7 ± 0.5 C C RJ7 ± 1.5 =•8.4 ± l c 9.6 ± 0.5 C 10.6 ± 0.5C 12.8 ± 0.5 C

(a) The first value is in agreement with the expected value for Kg = 4 . 1 . (b) At the R/Ro peak value the thermal coefficient is a little higher (30%) than the one reported in the literature (Kg = 2.0). (c) All the values, beyond the R/Ro peak, the thermal coefficient shows rapid increase.

408

H/Pd values reported in the table are taken from literature data up to R/RQ peak value and after this point we refer to Mc Kubre experimental and theoretical data, as previously reported. 12 In Fig. 3, we report known literature data ("+" points below the R/RQ peak) in addition to the new experimental data ("0" points beyond the R/RQ peak) which show the progressive increase of Kg as the H/Pd value increases (overloading); the arrows show the trend of Kg with increasing loading ratio. 14

14

•i

12 + r

1 0

CO

12 10 - ^

%

3 8 3

Q

y



3 2

- i — i . - L - i i ,...., I. .i

1

i.....J..t-1-j-U-,

1.11.21.31.41.51.61.71.8

Figure 3. P d - H temperature coefficient vs normalized resistance of the wire. Experimental data are reported in addition to literature data.

Similarly, in Fig. 4 we report data from the literature and the experiments; they show clearly the rapid progressive increase of Kg at H/Pd overloading. 3. Discussion 3.1. Phase

Hypothesis

From the literature, 2,3 ' 6 it is known that at room temperature the system Pd-Hx occurs in different phase conditions (a-phase at H/Pd = 0-0.1 and a + ft phase at H/Pd = 0.1-0.6). Because of the change of dimension occurring for R/Ro at the peak value of 1.8 when H/Pd is ranging from 0.7 to 0.8,1 it is possible to suppose a phase transition is taking place as it is pointed by an arrow in Fig. 1 at R/RQ = 1.7. At this R/RQ peak we hypothesize a new phase, named "/3 + 7" phase. If, at high H/Pd loading, this R/RQ peak is surpassed, we can assume that a peculiar 7-phase

409

^

I

-16

$

1

-

rn c —*: CD

Figure 4. P d - H temperature coefficient vs normalized H / P d loading. McKubre tables, are reported in addition to literature data.

Estimated data, from

occurs in correlation with the change of slope of the Kg vs temperature curve (Fig. 4) so that this new phase is peculiar of H/Pd high loadings.

3.2.

Conclusion

In conclusion, we stress the following points: • We are able to achieve H/Pd = 1 staying stable for a long time. • We can calculate Thermal Coefficient of Resistance at high Pd-H loadings. • At high loadings as the R/RQ strongly decreases, the thermal coefficient of electrical resistivity strongly increases. • We can conjecture a new important phase occurring at high loadings. Because all tests were performed using Hydrogen (i.e. light water) instead of deuterium (i.e. heavy water) we do not expect any anomalous heat in excess produced by the wire (i.e. Fleishmann and Pons effect), in fact we never detect thermal anomalies using light water in electrolysis solution. If such an anomaly occurred, wire temperature increasing (in respect to solution temperature) could alter the thermal coefficient measurement, but just this change of expected value could be an indication of anomalous excess heat.

410

Acknowledgments We are indebted to Eng. Alfredo Mancini for his precious support. We are grateful to Dr. Daniele Garbelli and Dr. Luca Gamberale for their important help and we want to t h a n k Dr. Mike McKubre for his useful suggestions. We like to stress the expertness of Mr. Vincenzo Andreassi, our skill technician. Appendix We used the known formula to calculate Kg: R(x,6)

= R0(x)(l

+ Ke{x)

9)

(A.l)

where R (in fl) is the electric resistance of the wire (related to a fixed x = H / P d loading ratio) and depending on the wire t e m p e r a t u r e 6 (in Celsius centigrade); RQ is the wire resistance at 0°C of t e m p e r a t u r e . Kg is the t e m p e r a t u r e coefficient of resistance (in ° C _ 1 ) . We consider Kg constant within a large range of temperature; indeed we have checked this constancy (within 5% of variation) from 200 K up to 373 K with a overloaded wire. References 1. M.C.H. McKubre et al., Frontiers of cold fusion, Proc. ICCF3, 1992, Nagoya, Japan (1993), p. 5. 2. B. Baranowski et al, J. Less Common Met. 158, 347 (1990). 3. B. Baranowski and R. Wisniewski, Phys. Stat. Sol. 35, 539 (1969). 4. A. Spallone, F. Celani, P. Marini, and V. Di Stefano, Experimental studies to achieve H/Pd loading ratio close to 1 in thin wires, using different electrolytic solutions, Proceedings of the 9th International Conference on Cold Fusion, "Condensed Matter Nuclear Science" (Edited by Xing Z. Li.), Beijing (China), May 19-24 (2002), pp. 319-322. 5. A. Spallone et al., An overview of experimental studies about H / P d over-loading with thin Pd wires and several different electrolytic solutions, Proceedings of the 11th International Conference on Cold Fusion (Edited by J.P. Biberian), Marseilles (France), Nov. 01-05 (2004). 6. J.C. Barton, F.A. Lewis, and I. Woodward, Trans. Faraday Soc. 59, 1201 (1963). 7. M.C.H. McKubre et at, Galorimetry and electrochemistry in the D / P d systems, Proceedings of the First Annual Conference on Cold Fusion, Salt Lake City, Utah, March 28-31 (1990). 8. P. Marini, A. Spallone etal., XXISecolo Scienza e Tecnologia, AnnoX (1), 34-41 (1999). 9. F.Celani, A. Spallone et al., High hydrogen loading of thin palladium wires through alkaline-earth carbonates' precipitation on the cathodic surface. Evidence of a new phase in the Pd-H system, INFN: LNF-00/006 (P), 6 Marzo 2000, To be published by Physics Letter A. 10. P. Tripodi, M. McKubre et al., Phy.Lett. A 276, 122-126 (2000). 11. L. Gamberale, D. Garbelli, and G. Piana, Measurement of Heat Capacity of PdHx, Proceedings of the 9th International Conference on Cold Fusion, "Condensed Matter Nuclear Science" (Edited by Xing Z.Li), Beijing, China, 19-24 May (2002), pp. 105-108. 12. M.C.H. McKubre (Data reported at the same Conference and Private Communications).

M A G N E T I C I N T E R A C T I O N OF H Y P O T H E T I C A L PARTICLES MOVING B E N E A T H T H E ELECTRODE/ELECTROLYTE INTERFACE TO ELUCIDATE EVOLUTION M E C H A N I S M OF VORTEX A P P E A R E D ON P d SURFACE A F T E R LONG-TERM EVOLUTION OF D E U T E R I U M IN 0.1M LiOD

HIROO NUMATA Tokyo Institute

of Technology, 1-12-1 O-okayama, Meguro-ku, E-mail: [email protected]

Tokyo 152-8552,

Japan

MASANOBU BAN Tokyo Metropolitan

Industrial

Technology Research Institute, Tokyo 115-8586, Japan

3-13-10

Nisigaoka

Kita-ku,

Long-term electrolysis for well-annealed thick Pd rod (9.0 mm <j>) in 0.1M LiOD was performed. Microscopic observation of a postelectrolysis Pd surface showed that long-term electrolysis did not result in any cracking but surface voids, two long faults, voids arranged in a straight line and peculiar surface traces: vortex. N-cycle model was developed to explain the cold fusion reaction and the related phenomena resulting in improved reproducibility of cold fusion experiments. An important process in that model is the motion of deuterium from a vessel to other ones, which might occur the observed vortex patterns on a postelectrolysis Pd surface. However, there has been remained unsolved yet a phenomenological explanation for the process of the vortex formation. The lattice gas cellular automata method was utilized for simulating a simple 2D flow with the boundary conditions incorporating the motion of the coincidental flow of the hypothetical particles. The vortex pattern was obtained behind the obstacle, though the axis appeared along the electrode surface. However, by comparing the vortex patterns obtained by the Lattice gas cellular automata method simulation and a postelectrolysis Pd surface the vortex with the leaned axis along the electrode can only be acceptable to describe the motion of the hypothetical particles. The vortex of the massive electron appeared to be modified by Lorenz force during traveling the interface assuming a 2D circular motion.

1. Introduction Ever since the announcement of Fleischmann and Pons, and Jones et al. of the generation of neutron and thermal energy accompanied with electrolysis on Pd in 0.1M LiOD, there still has been remaining the questions about the mechanism of the cold fusion reaction. What kind of phenomenon occurs when deuterium is absorbed in Pd metal by electrolysis is unknown, it is believed, is one of the reasons never expelled from the above doubt. Numata 1 , 2 ' 4 proposed a nuclear reaction cycle model (thereafter shortened to N-cycle model illustrated in Fig. 3) to explain the 411

412

miscellaneous phenomena accompanied with the cold fusion reaction as a multiple cyclic process, similar to a natural phenomenon. An important process in that model is the motion of the hypothetical particles from a vessel to other ones and/or to surface. Microscopic observation of a postelectrolysis Pd surface after long-term electrolysis for well annealed thick Pd rod in O.IM LiOD showed surface voids, two long faults, voids arranged in a straight line and peculiar surface traces: vortex. 4,5 Lattice gas cellular automata method (LGCA) numerical simulation of the motion of the hypothetical particles having large kinetic energy accounted for the vortex pattern appeared on a Pd electrode surface.6 Thus, such anomalous phenomenon was proved to really occur during the cold fusion experiments, however, there has been remained unsolved yet the motion of the hypothetical particles between the electrified and magnetized interfaces. Recently, Lewis7 comprehensively discussed ball lightning experiments (also EV markings in the same subject) showing the various holes, markings and tunnels including tornado associated with cold fusion and transmutation effects. The morphology of tornado looks like the vortex pattern well. Anomalous surface morphology like volcano was first reported by Oomori et al. on Au 8 and Toriyabe et al. on Pd 9 in light water electrical discharge experiments. These various anomalous traces, markings, etc. could be explained with magnetohydro dynamics and quantum mechanical consideration. Our research endeavors are rooted to give an atomistic understanding of processes that occur the vortex on a Pd electrode surface after long-term electrolysis in O.IM LiOD. In this paper the role of magnetic interaction with the emitted particles at the electrode/electrolyte interface will be discussed premising the motion of the hypothetical particles mass like vortex in the atmosphere. The experimental details of the appeared vortex and the results of fluid dynamics simulation and finite element method are described to elucidate the vortex formation mechanism at the interface. 2. Experimental 2.1. Long-Term Evolution of Deuterium Electrode in O.IM LiOD

on Thick Rod Pd

Cold fusion experiments at ambient temperatures have been conducted by electrolysis of heavy water on a Pd electrode or the other stable metals, e.g., Ni, Ti, and Au electrodes. In Fig. 1, the electrolysis equipment, especially the geometrical shape and arrangement of the electrode, the counter electrode and an electrolyte are shown, and the measurement systems with respect to excess heat, neutron emission, and an isothermal water bath are not drawn. Using a potentiostat (or current supply) a constant cathodic current was applied to a Pd electrode on which an evolution of deuterium gas was occurred. By continuing a state where deuterium is strongly absorbed in a Pd electrode, heat generation or emissions of neutrons or charged particles is observed. We successfully performed non-intermittent electrolysis for two and ca. 6 months with two experimental runs, referred to Exp. 1 and Exp. 2, respectively. The characteristics of the experimental apparatus and

413

1. Pd rod cathode 2. Anode 3.0.1M LiOD electrolyte 4. Double jacketed transparent quartz cell 5. Addition tube 6. Thermocouple 7. Guide for Deuterium gas 8. Guide for Oxygen gas 9. Circulating water inlet 10. Circulating water outlet 11 - Current supply

Figure 1. Schematic diagram of electrolytic cell for deuterium absorption on a Pd electrode in 0.1M LiOD.

procedures are: (1) cast rod Pd electrode, (2) thicker rod Pd electrodes (rods with 9 and 21 mm diameters 3,4 ), (3) preparatory gas phase absorption of D 2 (D/Pd 0.36), (4) increase in electrolysis current density in a form of stepwise, and (5) temperature cycling. The experimental runs were conducted twice in 0.1M LiOD by using the rod Pd electrodes with a diameter of 9 mm referred to Exp. I, 5 and a diameter of 21mm referred to Exp. 2. 3 , 4 The surface pretreatment and electrolysis conditions are shown in Table 1 and the results of neutron measurement are described elsewhere. 3,4 3. Results and Discussion Description with respect to microscopic observation of a postelectrolysis Pd surface is made with the result of Exp. 1. Figure 2 shows an optical micrograph of the transverse cross-sectional area (shown as rectangular in the left), where the sample was taken from the apex of the electrode, embedded in epoxy resin and lightly etched. Figure 2, on the right, shows a peculiar grain structure, quadrified by two straight grain boundaries. In metallographic aspect the specimen as a whole is consisted of columnar crystals: long prisms, which is supposed to be grown longitudinally along the electrode center (also see Fig. 4). However, this microstructure of the Pd Table 1. Run no.

Current (mAcm

First

0.05-40 40-500 40 40 40

Second Third Fourth

2

)

Experimental conditions of Exp. 1 Pretreatment Cast, 800°C anneal (lO-* 7 torr) Acid treatment Polishing, acid treatment, evacuation, and D2 gas charge Evacuation, polishing, and acid treatment Evacuation, polishing, and acid treatment

414

Gold plated titanium wire I Gold electric leading wire Cross sectional area of electrode

Teflon sheath

9Pd rod

Epoxy resin

*

TC

Figure 2. electrode.

Schematic of Pd electrode and optical micrograph of cross sectional surface area of

electrode is unexpected, since the temperature of the electrode and that out side of the counter electrode showed no significant change corresponding to heat bursts. Hence, this is well acceptable, only when the small heat evolution in the interior of the electrode lasted long time so as to promote abnormal grain growth. Coupland et a/.10 found the recrystalline grain near the area of electrical connection. Thus, during emission of neutron, the heat evolution in the interior occurred slowly showing the symmetrical crystal structure. Since the above result obtained by microscopic observation is not the in situ measuremnt, it is impossible to give an answer to the matter when such a microscopic structure appeared or to the time correlation with neutron count rate. However, it was possible to estimate such problems by an analogy with a natural phenomenon, as shown below.

•Reaction vessel: many regions surrounded by stained tough zone

Nuclear reaction cycle

Figure 3.

Schematic of a nuclear reaction cycle model.

415

3.1. Nuclear

Reaction

Cycle

Model

So far, endeavors have been exerted on understanding the individual phenomenon accompanied with the cold fusion reaction, which is a complicated phenomenon as a whole. Under such an idea, by considering phenomena as an energy engine, N-cycle model 1 - 3 was proposed from a point of view of its continuous operation (four reciprocating cycle). It consists of four sequential processes: intaking and compression-triggering-reaction-scavenging, taking into account of the correspondence to long-term electrolysis of a thick rod Pd (Fig. 3). The following two key points are beneficially realized: (1) enhanced reproducibility of the experiments resides in continuation of the cycle, (2) on systematic consideration the hindered factors might come to the surface. Let the correspondence be examined with the model in question to the phenomena of the experiment. In the absorption and compression processes of the reactants of the reaction (see Fig. 3), a barrier layer of deuterium migration by compression stress (also corresponds to the B side of the single-side electrolysis referred to the report 1 ' 2 ) is formed as absorption in progress, resulting in formation of a vessel composed of the interior and blanket as the barrier layer. In the compression process, the interior appears to make expansion owing to the continued absorption, i.e., a part of the generated deuterium is contributed to further slow absorption. However the compression pressure of the blanket brings a kind of enhanced pinch effect resulting in an increase of the internal pressure (in otherwise an increase in stress). In the reaction process a reaction should be caused by an external trigger that is applied to the inside (i.e., injection of high energy particles from the outside) or by an internal trigger. As an actual internal trigger, Cases I and II (also shown in the report 4 - 1 1 ) can be considered depending on a manner whether the role of the fault formation should be regarded as the final step of the reaction process or a reaction is induced by allowing the fault formation to provide the blanket with a path to expedite further absorption. 11 Very many holes concentrated on both the sides of the fault found in the experiment 4 were discharge ports of the reaction products in the process of scavenging. At this stage, discharge is made with the products of the reaction together with unreacting deuterium. 11 ' 12 In case of the internal trigger I, emission of the neutrons and charged particles at first occurs as a precursor phenomenon of the cold fusion reaction similar to an earthquake as listed in Refs. 1 and 2. Second, fault is formed simultaneously with reaction. In case of the internal trigger II, vessel is formed in the compression process, although the D/Pd ratio could be insufficient to the reaction. Therefore, fault is formed through a barrier layer (formation of this layer makes it for either absorption or desorption to occur), which allows the absorption to take an easy route. Thus, it is inferred that the D/Pd ratio is raised, resulting in occurrence of the cold fusion reaction. The resulting ca. 6% expansion confirmed during the first run (also see the left of Fig. 4 ) 1 - 4 suggests the occurrence of considerable internal pressure increase corresponding to the absorption/compression process of N-cycle model. Apart from the identification of the reaction vessels and emitted particles, the subsequent outflow

416

Top view of interface //~

~ N \ Simulate flow

He + 7, in fact, at all times, the dependence of the coupling to the electromagnetic field must be included. 23 Although this fact has been known since the early 1970s, it does not appear in conventional fusion literature because the d + d —> 4 He + 7 occurs at a rate that is ~ 107 times slower than the comparable rates associated with the dominant (d + d —> 3 H + p and d + d —> 3 He + n) reactions. On the other hand, the reverse reaction, 4 He + 7 —> d + d has been studied in detail. Here, it is known in fact, as opposed to the reaction involving the simple form, associated with Eq. (1), a comparable factorization between NF and EM wave functions is not possible because the associated dynamics requires detailed information 23 about the coupling of the EM interaction with the NF. Lindley misquoted this as well as a number of additional facts, including the nature of the d + d —> 4 He reaction, which he had not investigated, and the fact that d's have unit spin. Also, at the time, important information about the nature of products was not known. With hindsight, his comments illustrate a misunderstanding of fundamental aspects of many-body physics. In particular, although in 1989, Bose-Einstein condensates (BECs) had only been observed in natural processes in cryogenic environments, involving near absolute zero T in helium, noncryogenic procedures involving laser-cooling were being developed for creating BECs. Beginning in 1995, these procedures made it possible to dynamically create BECs. Since that time, not only has it become possible to create, manipulate, and alter BECs, using lasers but to artificially stimulate phase transitions, in which states involving an initial configuration of localized bosonic atoms (that remain confined in regions of space, defined by particular lattice sites in an optical lattice) into delocalized

435

(coherent) states in which the bosonic atoms exhibit the kinds of wave-like behavior, that we suggested might be relevant, are produced routinely. 2.2. A Meaningful Symmetry

Context for LENR

based on Broken

Gauge

Although Lindley was conceptually wrong, his use of Eq. (1) illustrates an important source of confusion: Eq. (1) is based on a number of assumptions involving length and time scale. In particular, the associated picture assumes that because nuclear reactions are initiated, with high energy, initially, the effects of EM can be ignored. In hot fusion, this makes sense since in hot fusion, a form of perfect "SU2 symmetry" can apply, in which it is never possible to distinguish between protons and neutrons. In the normal nuclear physics scenario, then, to have protons and neutrons close enough together for reaction to occur, it is assumed they occupy a state involving asymptotically free nucleons, in which effects of EM can ge ignored, as Giuliano Preparata emphasized. In fact, when additional symmetries are present, this picture need not apply. At noninfinite temperature and energy, residual EM interactions are present that break SU2 symmetry. In all situations, the process of lowering the energy requires loss of symmetry. This occurs because of a general requirement: The GS, by definition, to be stable, must have the smallest overlap with outside processes. When many particles are present, however, as opposed to a gradual reduction in symmetry, involving de-excitation between states, near the asymptotically free state (assumed as the initial state in nuclear physics), an entirely different situation can occur, provided the overlap process involves changes in momentum and energy, involving the EM interaction. In particular, as opposed to de-exciting an initial state, involving asymptotically free particles, an initial state involving potential nucleon overlap can form through an approximate symmetry, and the de-excitation process can result from an instability associated with the symmetry. Within this alternative context, as opposed to nuclear reaction being initiated from an extremely excited state, involving a small number of particles, a combined motion of many particles, at or near the GS configuration, can take place and lead to nuclear interaction. From this near GS configuration, as opposed to forms of interaction that couple the highest possible states of excitation with an effectively asymptotically free state, the de-excitation process can involve many particles that all have effectively the same energy and momentum, in a configuration in which all particles actually have negligibly small kinetic energy. An important symmetry that can cause this is associated with the peculiar limit (involving the kind of rigid-body, Mossbauer-like, Umklapp processes, alluded to above) in which many particles, at once, move rigidly, in such a way that the separation between any two particles remains the same. This can be accomplished through a second observation, made by Preparata: That the zero of momentum can be altered, dramatically, by a classical motion, involving many particles moving in a particular way. An important point that Preparata did not fully appreciate, however, is that it is never possible,

436

a priori, to constrain a collection of particles within a particular volume, in such a way that the locations of the particles can be identified. Because the velocity of any particular, rigidly moving configuration, relative to the velocity of a second rigidly moving configuration, can be continuously varied, a large degeneracy exists, in principle, associated with many, closely related, rigidly moving configurations. In fact, in the absence of charge accumulation at the boundaries of a solid, these different configurations are related, in principle, to each other through a (trivial) but continuously varying change in a particular parameter (the center-of-mass momentum) that can be related to the choice of gauge, 12 associated with the vector potential. As a consequence, the associated symmetry is referred to as gauge symmetry. In the limit in which this form of symmetry becomes dominant, asymptotically, in a sufficiently large solid, it is possible to require that far from the boundaries of the solid, effectively, in the evaluation of any relevant matrix element (associated with a particular many-body process), Eq. (1) remains valid for any configuration involving nucleons, provided no change occurs in the relative separation coordinate (r) between the center-of-mass (CM) coordinates of different charged particles (associated with the behavior of $ E M W ) m regions located far from potential overlap with NFs; while in regions where the relative separation in CM coordinates overlap with NFs, changes are allowed to take place, provided the resulting changes in momentum are all transferred to a total change in the CM momentum of the solid, through an Umklapp process. From such a starting point, Preparata's idea that many particles can move at once can be generalized: Instead of one configuration moving classically, with a single momentum, all possible configurations, in which each configuration is related to the others by a fixed difference in momentum, can be allowed to take place. In all relevant interactions, all momentum from a potential LENR can be transferred instantly 12 to the CM without altering the relative energy or momentum in interior regions where the EM interaction is dominant. Formally, this requires that energy and momentum are conserved, but how this occurs is ambiguous since it is not possible to determine the locations of the charged particles within a particular volume. Within the constraints of this limit, the form of separable wave function, involving Eq. (1), can be generalized: Instead of particular pairs of d's (as we initially suggested), associated with conventional fusion, at far separation (through $ E M ( r ) , where r is large, relative to NF overlap) or at near separation (where $ n u c (r) applies, at locations where r has overlap with NFs), each function $EM(»") or $ n u c (r)) can be interpreted as involving a collection of charged and neutral nucleons. The requirement that changes in the nuclear coordinates only alter the CM momentum, in turn, and not lead to changes in the relative separations between charged particles, in the interior (bulk-like regions 10 ' 12 ) can lead to particular selection rules. In particular, in the early stages of the development of the IBS theory, we suggested an approximate selection rule: That the dominant d-d reactions involve changes in wave function through variations in nuclear coordinates (and potential nuclear reactions) not alter the wave function

(2)

Issues

The models under discussion are relatively complicated, and it is appropriate to make use of all tools available to gain understanding of how the models work. In the case of the coupled oscillator and Dicke system, there is an interesting and relevant limit that we need to consider. In the limit that the number of oscillator quanta is very large, and also that the number of excited states of the two-level system is also very large, then it is possible to develop analytic solutions. For simplicity, we focus on a version of the model with single phonon exchange (777-2 = 1), in which case the limit of the coupled oscillator and Dicke model approaches Hr - • AEM

+ fnuon + gAE^

+

M + n odd. (4)

The associated eigenvalues are given by EMo,n0

= M0AE + n0fuj0.

(5)

Very similar eigenfunctions occur for M0 + n0 odd. One sees that in this limit, the coupled oscillator and Dicke system have a comb of eigenvalues spaced uniformly every HLOQ. 3.3. Static

Solutions

and

Derealization

We have an important analytic solution for the limit of the coupled model in which localized solutions occur. Specifically, this means that the system will develop fluctuations in n and M that are on the order of the coupling constant g. The coupling strength g is essentially the interaction matrix element divided by the transition energy. It can be on the general order of the number of receiver-side two-level systems (if we are able to arrange for half to be excited), since the underlying interaction strength per nucleus is probably on the order of a few MeV. Hence, the coupled system in this kind of model can be very strongly coupled, and fluctuations will be very large. For a net conversion of nuclear energy into phonon energy, simple fluctuations may not be helpful. We would like large numbers of oscillator quanta to be converted (probably more than g), not simply for the system to possess fluctuations. Consequently, we need to understand the connection between the eigenfunctions and the associated dynamics. For example, we would ideally like to see eigenfunctions that are localized around the constant energy line, and extend over large regions in (M, n) configuration space. Localized eigenfunctions represent the opposite. Some derealization can be obtained by working in a regime in which the coupling coefficients are not constant. For example, the time-independent Schrodinger equation for coupled two-level systems and oscillator can be written as

Ei>M,n

AEM

+ hio0n i>M,n + uU[S(S

+ 1) - M{M + l)](n + 1) 4>M+i,n+i

+ ^[S(S + 1) - M(M + l)]n V M + I , „

+ V[S(S + 1) - M(M - l)](n + 1) VM-i,n+i + y/[S(S + 1) - M(M - l ) ] n ^ M - l , n - l J-

(6)

446

30

c20 < 10

*

"-8

-

^

-

—

6

^

*

-

*

^

4

^

^

-

m

*

2

—

0

m

^

2

^

+

4

6

8

<M> Figure 3. Calculation of the spread in oscillator number A n (upper curves) and spread in Dicke number A M (lower curves) for the distinct even eigenfunctions with £ = 8, AE/fiwa = 15, and g = 1.5. A solitary point at M = 0 marks the analytic result for the localized Bessel function approximate eigenfunction.

In the large n limit, the coupling coefficients are nearly constant around M = 0, but they vary increasingly as one moves away from M = 0. Localized eigenfunctions are obtained near M = 0, but away the eigenfunctions become more delocalized. This is illustrated in Fig. 3 where we show the spread in oscillator number An as a function of the average Dicke number (M). Near M — 0, one sees that the spread in both n and M approach the constant g result, with minor deviations seen since the eigenfunctions extend slightly into regions where the coupling coefficient depends on M. Away from M = 0, one sees a significant spreading in n, which is an indication of derealization. The spread in M becomes reduced as the boundaries are approached. This result is interesting since it illustrates that if the local symmetry of the coupling constants is broken, that delocalization can result. Also, that the amount of delocalization is stronger the more that the symmetry is broken. However, the resulting eigenfunctions do not closely follow the constant energy line. For example, we illustrate in Fig. 4 a representative eigenfunction that is close to the M-boundary. One sees a relatively large spread in oscillator number. Such behavior is typical for coupled systems with a modest number of two-level systems.

3.4. System

Dynamics

We have done a significant number of simulations of the linearly coupled oscillator and Dicke model, from which some intuition has emerged. We see localized states

447

Figure 4. Example of eigenfunction for coupled two-level system and oscillator for large n limit. The vertical axis is the associated spin quantum number M, and the horizontal axis is relative oscillator number n = n - no-

that correspond to the analytic solutions discussed above, which are static. The coupled system is capable of large scale energy exchange between the two degrees of freedom, as is completely clear from the numerical results that we have seen (and is also completely clear from the literature on this kind of model). We can construct what amount to classical states of the system from a superposition of the eigenfunctions in the large n limit, and track the resulting dynamics (since wavepackets in the configuration space can keep their shape approximately). We see net motion that is oscillatory in the two dimensions, with wavepacket motion in M very roughly oscillatory with a frequency on the order of AE/li, and wavepacket motion in n with a frequency on the order of UIQ. We can understand the results in terms of simple notions of potential and kinetic energy in the (M, n) configuration space. In these simulations, the wavepacket moves from one position with an associated potential energy (AeM +frwoii),with the velocity of the wavepacket associated with the system kinetic energy. Hence, if the wavepacket follows a trajectory that goes between regions with different amounts of oscillator or Dicke excitation, because of the system kinetic energy the wavepacket. will shortly move on.

3.5. Slow

Dynamics

These complicated dynamics are interesting, but they do not correspond well to our intuition about how energy is transferred between the two degrees of freedom

448

in experiment. We seek slower dynamics in which the two-level system energy is transferred to the oscillator, which would correspond to eigenfunctions that lie along the constant energy line. We do not see such eigenfunctions in numerical simulations with a relatively small number of two-level systems, and modest integer ratio of oscillator energy to two-level system energy. If we tune the relative energies, we are able to match the eigenstate energies between neighboring eigenfunctions which differ in energy by one two-level system quantum. In this case, we observe a weak mixing which corresponds to a slow exchange between two-level and oscillator degrees of freedom. In the event that the associated coupling strength is on the order of the oscillator energy, we would expect to see free exchange of energy between the two systems at a maximum rate on the order of AEuo at threshold, and at higher rates for stronger coupling. Such a rate of energy transfer can be commensurate with experiment. It is also consistent with the energy exchange mechanism discussed in our ICCF11 proceedings, although the associated model would be more complicated. 4. Dynamics of Coupled Dicke Systems Based on the discussion above, we are motivated to consider a new kind of model to describe the dynamics of the D2 system and the coupled receiver system. If we assume that significant conversion of excitation on the receiver side to phonons is slow, then it seems productive to neglect it completely in order to develop a description of the excitation transfer dynamics associated with the populations. There is the question of resonance. On the one hand, there is no reason to expect there to be receiver nuclei transitions that are matched to the energy difference between D2 and 4 He. On the other hand, there is no excitation transfer between unmatched Dicke systems in the limit of hindered coupling and no phonon exchange. This sharply limits the possibilities. If the energy of the nuclear excitation is fixed and off of resonance, then the energy difference must be made up through phonon exchange in the strongly coupled oscillator and Dicke system on the receiver side. Alternatively, it may be the case that the nuclear excitation energy on the receiver side is determined by the energy involved in the excitation transfer. The argument in support of this is that one would expect the nuclei to have a very broad energy response (perhaps roughly proportional to the giant dipole response, but not the same since our excitation is not dipolar) under the conditions of excitation transfer. After all, if a quantum of energy is transferred, and if the nuclear system does not lose the energy, then it should be available for transferring back. Overall in this scenario the transfer process would create a precise resonance. From our perspective, either scenario is consistent in principle with the discussion which follows. There is a price to be paid, however, if the energy difference must be made up by phonon exchange. That price is a substantial reduction in efficiency, since it would be that the associated "oscillator strength" of the hybrid system must have a large energy spread.

449

4.1. Evolution

of Resonant

Coupled Dicke

Systems

Excitation transfer between resonant Dicke systems is governed by the Hamiltonian

H = — £ « + —S&

-e-G sPsW + sVs™

+

(7)

The development of evolution equations for expectation values of the pseudospin operators is nontrivial in the general case. We have had success developing an approximate Ehrenfest calculation by adopting a restricted basis composed of degenerate states. The results of the Ehrenfest analysis, augmented empirically with loss, results in the following coupled equations:

~ni(t)

= Vl(t),

d .. n2(t) ^n2(t) + - ^ i

,. = v2(t),

^jUi(t) + ^

= a(t),

d , . V2(t) -v2(t) + -^=

-ait),

(8)

(9)

where a

W =

p

{ [Nl ~ Mt)\[N2 ~ n2(t)][n2(t) - nx(t)] +ni{i)n2{t)[Nl

- ni(i) - N2 + n2(t)]

+ [Ni - rn{t)]n2{t) - [N2 - n2(t)]m(t)\.

(10)

Here n\{t) and n2(t) are the average number of excited states in system 1 (D2 side) and system 2 (receiver side), and v\{t) and v2{t) are the associated velocities. The acceleration is a{t). The Dicke number for the two sides are iVi and N2l which can be as large as the total number of nuclei involved on each side.

4.2.

Example

In Fig. 5 we show results from a numerical calculation of the evolution equations for resonantly coupled Dicke systems. In this calculation, we have assumed that there are 10 times more receiver side nuclei in the ground state than there are D2 molecules in the upper state. In addition, we have set the relaxation time to be matched to the coherent transfer rate. If we use a much slower relaxation time, then we observe population returning from the receiver side. If we use a much faster relaxation time, then we observe a slower net transfer of excitation. The problem in this case is that if the receiver-side nuclei decay rapidly, then there are relatively few around to provide a (receiver-side) Dicke enhancement of the acceleration. In essence, the fastest net energy generation rate is obtained when we match the excitation transfer rate with the receiver-side loss.

450

10

30

20 12

_G

(2A/1A/2) ' V e f / h b a r Figure 5. Calculation of normalized populations x(t) = ni(t)/Ni function of normalized time for conditions in which N2 = 10N±.

and y(t) = ri2(t)/N\

as a

5. Avoidance of Loss We have noted previously that the probability amplitude tends to avoid regions of high loss. A very much simplified version of this argument can be given. Consider the situation of two states that are coupled, one loss free and the other with high loss: d ih—co(t)

= flocoW + V&icift), .fill

Hi

ci(t) + Vi0co(t).

(11) (12)

We initialize the system such that c0(0) = 1, and ask what happens later on. The exact solution is more complicated than what we are interested in here; however, a useful simplification is allowed if we assume that the level 1 loss is very strong. In this case, CQ decays slowly as we will find, and we may assume that the a(t) probability amplitude is determined in the steady state by Cl (t)

E-

Hx+ih-a/2

VLO

c0(t)

(13)

with E approximately H0. The resulting evolution of level 0 is then

^

( t )

= W )

+

F&^

(14)

451

The effective loss seen by level 0 is then =

[Vbil2

'

n

,.

Increasing the level 1 loss 71 to ever larger values has the perhaps unexpected effect of decreasing the level 0 loss. In essence, the probability amplitude tends to avoid level 1 as it gets increasingly lossy. Alternatively, one can view this result as indicated that the maximum loss from level 0 is obtained when the loss is matched to the coherent transition rate.

6. Nuclear Models We have made progress on the other half of the problem which involves the calculation of the nuclear response in the presence of phonon-mediated excitation transfer. The calculation of phonon exchange matrix elements requires the inclusion of the nuclear center of mass coordinates as phonon operators. Results relevant to such calculations for the four-body problem is discussed in another paper submitted to this proceedings.6 We have in addition developed a new strategy for the calculation of the nuclear response which may be worth discussing briefly. The lattice generalization of the resonating group method that we have developed allows us to include phonon exchange explicitly in calculating nuclear interaction matrix elements. It seems that the most relevant and perhaps cleanest calculation which is needed is a second-order process in which an initial nuclear system receives energy via excitation transfer in a first phonon mediated strong force interaction, then evolves as a daughter plus neutral, and after a while makes a transition to a final state nuclear system. The basic interaction matrix element can be represented as

Mfl(E)

J2(^f(^f(^'---^A)\VN\^>mt[E-Hmt}-1

= int

x{*int\VN\MZu---,U)*i{ 4 He on the D 2 side, as well as AZ —> n m + A _ m Z —> A Z transitions on the receiver side. The matrix element can be represented by a Feynman-like diagram that is illustrated in Fig. 6. Implicit in the expression for the matrix element and also in the diagram is the point of view that the lattice (or condensed matter system) separates from a neutral (in association with an excitation transfer event), evolves as a daughter lattice plus neutral in the intermediate state, and then comes back together to form the final state lattice. Instead of a vacuum language that focuses on nuclei and nucleons, in the formulation under discussion, the interaction is with a nuclei which is part of a lattice, and it is helpful to think of it as a neutral plus lattice separation. Such a view makes plain what the calculation involves at the outset, and makes clear that it is in fact a fundamentally different calculation than what is involved in related vacuum calculations. 7. Summary We are moving toward viewing relevant models as involving the hindered coupling between a Dicke system for the D2/ 4 He side and a hybrid quantum system on the receiver side composed of one or more Dicke systems strongly coupled to one or more highly excited oscillators. In previous work, we have discussed the possibility that loss can break the symmetry of the coupled oscillator and Dicke Hamiltonian in order to allow the conversion of nuclear energy to phonon energy. Here we have shown that

453 the n a t u r a l boundaries associated with the Dicke system can accomplish the same basic function in a relevant strong coupling limit. Energy transfer between the Dicke system and the oscillator can occur naturally on timescales of the oscillator and two-level system generally in coupled Dicke oscillator systems. In strongly coupled systems in which the coupling strength between nearly degenerate eigenfunctions exceeds the oscillator energy, free energy exchange is expected. This corresponds to the situation we expect in the case of coupling between receiver nuclei and a highly excited acoustical phonon mode. It also is closely related to the coupling mechanism we discussed in the I C C F l l proceeding for a closely related model of two Dicke systems coupled to an oscillator with different coupling strengths in the classical limit. We presented the results of an Ehrenfest analysis of coupled resonant Dicke systems, augmented with loss to take into account energy coupling with the lattice in an empirical way. T h e resulting evolution equations should be relevant to the dynamics of fusion reactions under conditions where the D2 source is not replenished. Progress on the nuclear calculations was discussed briefly as well.

References 1. M. Fleischmann, S. Pons and M. Hawkins, J. Electroanal Chem. 201, 301 (1989); Errata, 263, 187 (1990). See also M. Fleischmann, S. Pons, M.W. Anderson, L.J. Li and M. Hawkins, J. Electroanal. Chem. 287, 293 (1990). 2. S.E. Jones, E.P. Palmer, J.B. Czirr, D.L. Decker, G.L. Jensen, J.M. Thorne, S.F. Taylor and J. Rafelski, "Observation of cold nuclear fusion in condensed matter," Nature 338 737 (1989). 3. P.L. Hagelstein, Proceedings of the Ninth International Conference on Cold Fusion, May 2002, Beijing, China, in: X.Z. Li (ed.), p. 121. 4. P.L. Hagelstein Proceedings of the Tenth International Conference on Cold Fusion, Aug. 2003, Cambridge, MA, in: P.L. Hagelstein and S.R. Chubb (eds), p. 837. 5. P.L. Hagelstein Proceedings of the Eleventh International Conference on Cold Fusion, Nov. 2004 Marseilles, France, in: J.P. Biberian (ed.), (in press). 6. I. Chaudhary and P.L. Hagelstein, this proceedings.

T I M E - D E P E N D E N T E Q P E T ANALYSIS OF TSC

AKITO TAKAHASHI1 Osaka

University,

Yarnadaoka 2-1, Suita, Osaka 565-0871, e-mail: [email protected]

Japan

Time-dependent fusion rates for 2D and 4D reactions are calculated for squeezing of tetrahedral symmetric condensate (TSC) from about 100 pm size to its minimum size (about 10 fm), within about 75 fs squeezing motion. Life time of the minimum TSC state is yet to be studied. Time-averaged fusion rates are given by assuming the life time of minimum TSC state is negligible. Time-averaged 2D fusion rate was given as 2 . 9 x l 0 ~ 2 6 f/s/pair, and time-averaged 4D fusion rate was 5 . 5 x l 0 - 8 f/s/cl. These values are compared with 1.0xl0~ 2 0 f/s/pair for 2D and 1.0 X 1 0 - 9 f/s/cl for 4D, respectively, of previously estimated values by electronic quasi-particle expansion theory/TSC m o d e l s . 1 _ 3 Effective fusion time by the TSC squeezing motion was estimated as 0.04 fs: namely fusions may happen in very short time interval.

1. Introduction For a consistent theoretical model of various condensed matter nuclear effects, namely clean 4 He producing fusion and cold transmutation, electronic quasi-particle expansion theory (EQPET)/tetrahedral symmetric condensate (TSC) models have been developed by the author. 1_4 Transient motion of TSC by four deuterons plus four electrons has been treated with a primitive approximation using the linear combination (EQPET) of wave-functions for pseudo-molecular states of d-d pairs with normal electrons and quasi-particle-electron states e*(2,2) and e*(4,4) as steadystate solutions for narrow time-window. This was a model for "bosonized condensate" of squeezed mode, which can be treated as a kind of steady state in very narrow time-window of squeezed motion. Since the barrier factor changes drastically with astrophysical orders according to the assumed pseudo-molecular states, numerical studies based on time-dependent treatment are expected to know more accurate values of fusion rates of multi-body deuteron interactions in the transient process. This work reports a trial study of time-dependent EQPET analysis for TSC squeezing motion to estimate time-averaged fusion rates of 4D/TSC.

tSubmitted to ICCF12, November 2005. 454

455

2. E Q P E T Model Starting with the formation of TSC state (t = 0) with six-wings wave function which is composed of six dde* molecular wave functions with six orthogonal single spin wave functions, time-dependent screening potentials are adiabatically approximated with pseudo-molecular potentials for ddee, dde* (2,2) and dde*(4,4) according to the change of mean d-d distance i?dd- Semi-classical treatment is done for the timedependent reduction of mean d-d distance. Using this algorithm, a computer code is made.

4re = 4x2.8 fm

(2) Minimum TSC

(1) TSC forms Electron

r~\





> 4

4

He

He

Deutron 15fm

(3) 8 Be* formation Figure 1.

(4)

Break U

P

Four steps for TSC squeezing motion and 4D fusion.

The semi-classical feature of TSC squeezing motion is illustrated as four steps in Fig. 1. In Fig. 1, TSC will form in the near surface region of condensed matter by the mechanism (A) or mechanism (B) as discussed in Refs. 2 and 3, with certain probability depending on methods of experiments and near-surface physics of condensed matter. Step 1 (TSC forms). Then TSC starts Newtonian squeezing motion to decrease linearly its size from about 100 pm radius size to much smaller size and reaches at the minimum size state. Step 2 (minimum TSC). Classical squeezing motion ends when four deuterons get into the strong force range (5fm) and/or when four electrons get to the Pauli's limit (about 5.6fm for e-e distance). Here for

456

the Pauli's limit, we used the classical electron radius of 2.8 fm. In Step 3, mutual charged-pion exchange between four deuterons forms 8 Be* intermediate compound state with much smaller radius and the charge neutrality in average of 4D/TSC is broken simultaneously to kick out four electrons. In Step 4, 8 Be* which is collectively deformed with two alpha-clusters promptly breaks up to two 4 He particles. The initial state TSC wave function, when TSC is just formed at t = 0, can be written using combination of six wings of D2 molecule wave functions on six surfaces of the TSC cube, as illustrated in Fig. 2. Here, the wave function of D2 molecule is written with combination of two 1 S wave functions \&ioo of hydrogen atom, as also illustrated in Fig. 2. This feature is obtained by assuming the TSC wave function to be the following Eq. (1) and using the three-dimensional symmetric constraint of TSC squeezing motion in applying the quantum mechanical variational principle of minimizing system energy. The new aspect of the problem is that we are treating "bosonized condensate" of TSC under the environment of ordered dynamic motion (in other words, symmetrically constrained squeezing motion) in the lattice of PdDx condensed matter. *4D ~ ai[^ r 100(''Al)*100(''B2) + *10o(r - A2)*10o(r 1 Bl)]^"s(5'l, 5 2 ) + a2[*100(^Al)*100(^D4) + *10o(rA4)*10o(n3l)]-Xs(£i,S4) + a3[*100(»,A2)*100(»,C4) + *100(jA4) , I'l00(7C2)]^s(S , 2, S4) + a 4 [*100(»'Bl)*100(rD3) + *100(?~B3)*100(>'Dl)]^s(<Sl,S'3)

+ a5[*ioo(^B2)*ioo(»'C3) + ^ioo(rB3)^ioo(rG2)]Xs(S2, + a 6 [*ioo(rc3)*ioo(r D 4) + ^wo{rc4)^wo(rD3)}Xs(S3,Si)

S3) (1)

and the 1-s electron wave function for deuterium atom is given by, *ioo(r) = ( l A ) 1 / 2 ( l / a B ) 3 / 2 e x p ( - r / a B ) .

(2)

Here subscripts A-D denote positions of deuterons at vertexes of cube. And subscripts 1-4 denote positions of four electrons. XS(S{, Sj) is singlet spin wave function for bosonized (anti-parallel spins) pair of electrons. Bohr radius ae is 52.9 pm. Coefficients a\-a% are vectors on six surfaces of the cube, and are usually determined by the variational method to minimize system energy as, <S{/} = 0.

(3)

Since the solution of Eq. (3), with partial derivatives for coefficients a\-a§, gives sixth order (18th order in exact, taking three-dimensional components of vector aj) secular equation which cannot be solved uniquely. However, the requirement of ordered squeezing, namely the three-dimensionally symmetric constraint of TSC motion in PdDx lattice, gives constraints as,

Kl = Kl = M = M = \a5\ = \a6\ = a0 with a0 = 1/(6(1 + A)) 1 / 2 .

(4)

457

Feature of QM electron cloud Electron center; <e> = (et + ie)/2

RB = 53 pm

• Bohr orbit of D (H)

Deutron

(a) D atom (stable) Bosonized electron center torus for (et + 4e)

y - i^m. *^ y

v_y

Orbit of bosonized electron coupling for (et + ie)

/

(c) 4D/TSC (life time about 60 fs) 73 pm (b) D2 molecule (stable): V 2 D = (2+2Ar 1/2 [ Vl00 (r A1 ) ¥ioo(%z) + Vioot'Aa) ¥IOO('BI)]^S(SI. S2) Figure 2. Features of QM electron clouds for (a) D atom, (b) D2 molecule, and (c) 4D/TSC at t = 0. Bosonized electron center torus of D 2 molecule is a unit of bond for orbits of bosonized electron coupling of TSC (t = 0).

And we have orthogonal conditions between a4 for i = 1-6. aiaj=%.

(5)

We can say that the platonic polyhedral symmetry in constraint motion gives special solution for the variational analysis of so-many-body problem. Thus the TSC wave function at t = 0 has six symmetric wings of modified D 2 wave functions as illustrated in (c) of Fig. 2. D 2 wave function has a torus of electron higher density for singlet (anti-parallel) spin pairs of electrons. Superposition of "wings" at vertexes of the cube make four balls of high density electron clouds at tetrahedral four vertexes of cube as illustrated in Fig. 2c. An electron ball at vertex can be therefore treated as an effective electron center for (e) = ( e | + e|)/2. In Fig. 1, we have drawn effective electron center as classical electron particle with spin. 3. Time-Dependent E Q P E T Analysis The basic equation of time-dependent EQPET is written as *4D(r, t)at = a i ( t ) * ( l , l)(r, t) + o 2 (t)*(2,2)(r, t) + a 4 (t)¥(4,4)(r, t),

(6)

(r(t)) = - (v)t,

(7)

458

M*)} = ,

(8)

(r(0)) = (3 1 / 2 /2)a B = 45.8 pm.

(9)

Here we assumed that the time-dependent 4D/TSC wave function ^4u(r,t) can be expanded with the linear combination of time-dependent wave functions * ( l , l ) ( r , £ ) , #(2,2)(r,t), and *(4,4)(r,i) of EQPET molecules1-4 dde(l, l)e(l, 1), dde*(2,2) and dde*(4,4), respectively. Eq. (7) assumes classical Newtonian motion treatment for averaged particle position with strong constraint of same velocity due to keeping charge neutrality (system Coulomb energy to be minimum) in TSC squeezing motion. Modal fusion rate 5 for 4D cluster is given as A„d(*) = ai(t) 2 A„ d (l, l)(t) + a 2 (i) 2 A„ d (2,2)(t) + a 4 (t) 2 A„ d (4,4)(i).

(10)

Here we take n = 2-4 for 4D/TSC cluster fusion rates. Fusion rates for an EQPET molecule are given by Xnd{m,Z)(t)

= (vSnd/Ed)Pnd(Ed,t).

(11)

Here v is the relative deuteron velocity, Snd the astrophysical S-value (intrinsic cross-section term for strong interaction) for multi-body fusion and Ed the relative deuteron energy, respectively. Also we define the time-dependent barrier penetration probability Pnd(Ed,t) as follows: Pnd(Ed,t)=exp(~nr{t)),

(12)

T{t) = 0.218 / y/Vs(Rdd) - Ed dRdd (in MeV and fm unit). (13) Jr0 Here Rdd is the inter-nuclear distance between two deuterons. For evaluating the time-dependent Gamow integral Eq. (13), we employed the adiabatic approximation for time-dependent potentials for EQPET molecules using three steady-state potentials 6 Vs(Rdd) for (1,1), (2,2), and (4,4) state-electron couplings. Major parameters of EQPET molecule potentials are shown in Table 1. The algorithm of adiabatic treatment is as follows: b{t) = Rdd(t) = bo(m,Z)

forVs-Ed>0 forVs-~Ed (pm) Time (fs) 72.98

Figure 3.

72.9

Calculated time-dependent cluster fusion rates for TSC squeezing motion.

We found time-averaged 2D fusion rate 2.9 x 10~ 25 f/s/pair is about five orders of magnitude smaller than the steady squeezed mode analysis, but time-averaged 4D-fusion rate 5.5 x 10" 8 f/s/cl is rather closer value. Of course we should prefer values by the present time-dependent analysis. 5. Conclusions 1. Simplified trial of time-dependent analysis on TSC was made. 2. TDEQPET (time-dependent code) gave several orders of magnitude different fusion rates from those by EQPET (Squeezed Mode Model). 3. 4D fusion takes place in 0.04 fs effective reaction time: It is very impulsive. 4. TSC as bosonized condensate has been proposed as SEED of Condensed Matter Nuclear Effects to induce clean 4D fusion. Table 2. Time-averaged modal fusion rates and initial fusion rates for 4D/TSC squeezing motion, calculated by T D E Q P E T code T D E Q P E T calculation for E Q P E T molecules

e*(m,Z)

(A2d) (f/s/cl.)

(A4d) (f/s/cl.)

A2d(0) (f/s/cl.)

A4d(0) (f/s/cl.)

(1,1) (2,2) (4,4)

4.3 x 1 0 " 4 4 2.9 x 1 0 " 2 5 (2.1 x lO" 17 ) 1 "

7.8 x l O - 6 3 2.5 x 1 0 - 2 4 5.5 x 1 0 " 8

1.9 x 1 0 - 6 0 2.4 x 1 0 - 3 7 (5.5 x l O - 2 2 ) !

7.3 x 1 0 ~ 9 3 1.1 x 1 0 " 5 0 5.9 x l O " 2 0

t Virtual value.

461

References 1. A. Takahashi, Deuteron cluster fusion and related nuclear reactions in metaldeuterium/hydrogen systems, Recent Research Developments in Physics, Transworld Research Network, India, 6, 1-28 (2005), ISBN = 81-7895-171-1. 2. A. Takahashi, TSC-induced nuclear reactions and cold transmutations, Siena Workshop on Anomalies in D/H loaded metals, Siena, Italy, 13-16 May (2005), http://www.iscmns.org/. 3. A. Takahashi, A theoretical summary of condensed matter nuclear effects, ibid. 4. A. Takahashi, Condensed Matter Nuclear Effects, Proc. IMFP2005, Int. Meet. Frontiers Physics, 25-29 July (2005), Kuala Lumpur, Malays. J. Phys., to be published. 5. A. Takahashi, Mechanism of deuteron cluster fusion by EQPET model, Condensed Matter Nuclear Science, Proc. ICCF10, World Scientific Publ. Co., pp. 809-818 (2006), http://www.lenr-canr.org/. 6. A. Takahashi, Drastic enhancement of deuteron cluster fusion by transient electronic quasi-particle screening, Proc. JCF4, pp. 74-78, A. Takahashi, Deuteron cluster fusion and ash, Proc. Asti Workshop (2004) http://www.iscmns.org/.

U N I F Y I N G T H E O R Y OF L O W - E N E R G Y N U C L E A R R E A C T I O N A N D T R A N S M U T A T I O N PROCESSES IN D E U T E R A T E D / H Y D R O G E N A T E D METALS, ACOUSTIC CAVITATION, GLOW DISCHARGE, A N D D E U T E R O N BEAM EXPERIMENTS Y E O N G E. K I M A N D A L E X A N D E R L. Z U B A R E V Department E-mail:

of Physics, Purdue University, 525 Northwestern Avenue, West Lafayette, IN 47907, USA [email protected]; [email protected]

The most basic theoretical challenge for understanding low-energy nuclear reaction (LENR) and transmutation reaction (LETR) in condensed matters is to find mechanisms by which the large Coulomb barrier between fusing nuclei can be overcome. A unifying theory of LENR and LETR has been developed to provide possible mechanisms for the LENR and LETR processes in matters based on high-density nano-scale and micro-scale quantum plasmas. It is shown that recently developed theoretical models based on Bose-Einstein Fusion (BEF) mechanism and Quantum Plasma Nuclear Fusion (QPNF) mechanism are applicable to the results of many different types of LENR and LETR experiments.

1. Introduction There have been many reports of experimental evidences for low-energy nuclear reaction (LENR) processes in condensed matters as documented in a recent document submitted for a DOE review1 and as reported in Proceedings of ICCF-10. 2 However, most of experimental results cannot be reproduced on demand. This situation has prevented us from development of a coherent theoretical understanding or working theoretical model of the phenomenon which can be used to guide us in designing and carrying out new experimental tests to sort out essential parameters and controls needed to achieve reproducibility on demand (ROD). In this paper, it is shown that recently developed theoretical model based on Bose-Einstein Fusion (BEF) mechanism and Quantum Plasma Nuclear Fusion (QPNF) mechanism are applicable to the results of many different types of LENR and transmutation experiments. Both the BEF and the QPNF mechanisms are based on a same physical model, which assumes that deuterium/hydrogen is in a plasma* state and is mobile in a deuterated/hydrogenated metal as deuteron/proton ion.t *In this paper, we use a general definition of "plasma" as given in the report: National Research Council, "Plasma Science", National Academic Press, Washington DC (1995), p. 1, "Plasma science is the study of the ionized states of matter". * Experimental evidences for the ionization and mobility of deuteron/proton in metal are given in Refs. 14-16. 462

463

Theoretical studies of BEF mechanism have been carried out using an approximate solution to the many-body Schroedinger equation for a system of N identical charged, integer-spin nuclei ("Bose" nuclei) confined in micro- and nano-scale cavities. 3-6 The ground-state (superfluidity state) solution is used to obtain theoretical formulae for estimating the probabilities and rates of nuclear fusion for N identical Bose nuclei confined in a ion trap or an atomic cluster. Most recently, we have investigated the effect of a generalized particle momentum distribution derived by Galitskii and Yakimets (GY) 7 on nuclear reaction rates in plasma. 8 ' 9 We have derived an approximate semi-analytical formula for nuclear fusion reaction rate between nuclei in a plasma. The formula is applied to calculate deuteron-deuteron fusion rate in a plasma, and the results are compared with the calculated results of the conventional Maxwell-Boltzmann (MB) velocity distribution. As an application, we investigate the deuteron-deuteron fusion rate for mobile deuterons in a deuterated metal/alloy. The calculated deuteron-deuteron fusion rates at low energies are enormously enhanced due to the modified tail of the GY's generalized momentum distribution. Our preliminary estimates indicate also that the deuteron-lithium (D + Li) fusion rate, the proton-boron (p+B) fusion rate, and the proton-lithium (p + Li) fusion rate in a metal/alloy at ambient temperatures are also substantially enhanced due to this QPNF mechanism. Implications of our results and other potential applications are discussed. 2. Bose-Einstein Fusion (BEF) Theoretical studies of the BEF mechanism are described in publications 3-6. One of the main predictions is that the Coulomb interaction between two charged bosons may be suppressed for the large N case and hence the conventional Gamow factor may be absent. The theory has been used to analyze LENR experiments involving both atomic clusters (Pd black powders 10 ) and acoustic cavitations. 11 Recently, the one-specie LENR theory of the BEF mechanism 3-6 used for reactions such as (D+D) has been generalized to the two-species case and applied to (D + Li) reactions. 12 The only unknown parameter of the theory is the probability of the BE groundstate occupation, ft. Since, ft is expected to increase as the effective temperature of the BE state (superfluidity state) decreases, the nuclear reaction rates for the BEF mechanism are expected to increase at lower temperatures. 3. Quantum Plasma Nuclear Fusion As shown by Galitskii and Yakimets (GY), 7 the quantum energy indeterminacy due to interactions between particles in a plasma leads to a generalized momentum distribution which has a high-energy momentum distribution tail diminishing as an inverse eighth power of the momentum, instead of the conventional MB distribution tail decaying exponentially. GY's generalized momentum distribution has been used by Coraddu et al.13 in an analysis of anomalous cross-sections for D(d,p) 3 H observed from the low-energy deuteron beam experiments.

464

In this section, we describe a QPNF mechanism, which includes the effect of GY's generalized momentum distribution on the nuclear fusion rates in a plasma. 8 ' 9 The calculated results based on the QPNF mechanism for deuteron-deuteron fusion rates are compared with the results of the conventional calculation with MB distribution. As applications of the QPNF mechanism, we investigate other nuclear fusion rates for (D + Li), (p + Li), and (p + B) reactions in metals/alloys. 3.1. Reaction

Rates for Quantum

Plasma

Nuclear

Fusion

To formulate the QPNF mechanism we start with GY's generalized distribution function given by f(E,p)=n(E)S1(E-ep),

(1)

where n(E) is MB, Fermi-Dirac (FD), or Bose-Einstein (BE) distribution, modified by the quantum broadening of the momentum-energy dispersion relation, 57(E — e p ), due to particle interactions. 51(E — ep) is given by

^

£p)

{Z)

-irl(E-Sp-A(E,p)y+1i(E,p)Y

where e p = p2/2/x is the kinetic energy in the center of mass coordinate of an interacting pair of particles, u is the reduced mass, A(E,p) is the energy shift due to the interaction (screening energy, etc.), and j(E,p) is the line width of the momentum-energy dispersion due to collision. ^{E^p) RJ hpcac^2E/n, where pc is ( 2 2 2 the number density of Coulomb scattering centers (nuclei), ac = Tr(ZfZ je ) /s is the Coulomb scattering cross section, and Zfe is an effective charge which depends on e p . For small values of e p , Zf is expected to be much smaller than Z*, Zf 0 and 7 ->• 0, S1(E-ep)

= S(E-sp).

(3)

The nuclear fusion rate for two nuclei is given by ( kT, 7 and A we obtain approximately /(fl«l

fn(E)1(E,p)dE

= rJ81^Pc{Z!Zle2)2 7T^ '

j

£4

ocl, po

(7)

465

as shown by GY. 7 This is to be compared with the other conventional cases, f(p) oc e~ £p / fcT . We now derive an approximate analytical formula for obtaining order-ofmagnitude estimate for the nuclear fusion rate. The total nuclear fusion rate, R^, per unit volume (cm - 3 ) and per unit time (s _ 1 ) is obtained from an expansion of Eq. (2) in which the first term is S(E — e p ). R^ is approximately given by Rij « Rtj + Rtj,

(8)

where i?£ is the conventional fusion rate calculated with the MB distribution and i O is the contribution from the second term of the expansion of Eq. (2) and is given by

Gr

where EQ is the Gamow energy, EQ = (2-KaZiZj)2/j,c2/2, p± is the number density of nuclei, and S'ij(O) is the S'-factor at zero energy for a fusion reaction between i and j nuclei. We note that the spectral function 5-y{E — ep) (Eq. 2) introduced by GY 7 needs to be modified to satisfy the following energy weighted sum rule (for fermions),

jMES^E-eJ-^-JW^M,

(10)

where f(p) is the distribution function, given by Eq. (5). Since the integral on the left-hand side of Eq. (10) is a divergent integral, the GY parameterization of ~f(E,p) in 81(E — ep) needed to be corrected for large £ >fcTto satisfy the above sum rule. However, Eqs. (4-9) are still valid since our results for the distribution function f(p) do not depend on j(E,p) in the region where E 3> kT due to the presence of n(E) oc e~E/kT in Eq. (5). 3.2. (D + D) Reactions

in a Plasma

The importance of Eq. (9) is that it distinguishes high density/low temperature plasmas in condensed matter systems from low density/high temperature plasmas produced in magnetic confinement plasma fusion or inertial confinement laser fusion by breaking the contribution of fusion reactions into the MB and the QPNF processes. To access the importance of each, it is useful to investigate the cross section times the velocity averaged over the velocity distribution or fusion reactivity (av), given by Eq. (9), as a function temperature. In Fig. 1, the calculated fusion reactivities, (o~v), are plotted as a function of temperature kT. There are two density regions of interest; the hydrides in metals shown as the solid line in the figure and the tokamak break-even density shown as the dotted line in the figure. The fusion reactivity of a MB distribution is independent of density and is shown in the figure as a dashed line. The intersections of the dashed curve and the solid or dotted curves provide values of critical temperature T cr ,

466

10- 27

—

-'—

-—v.-f

_

Condensed matter p QPNF-theory

10-29

/ / I I I i

b

icr 33

•S co

10-35

c

1(T

Tokamak p-goal QPNF-theory

?

' j

/

I

, * m 1 when there is no absorption. It means a constructive interference among all the propagating waves inside A^-layers, which enhances the penetration rate greatly. The conservation of the probability guarantees the eventual penetration after all the reflections and penetrations in layers. Now we may introduce a small absorption coefficient, A(l) < (3TT/8), the three total coefficients are oscillating, b u t beyond this interval, they are decaying or growing monotonically. This behavior is expected from the coherence as well. T h e phase angle, a in Eq. (8), includes b o t h the information for single layer (A(l)) and the information for multiple layer(0). W h e n A(1) —> 0, cos a in Eq. (7) is mainly a real number. However, a may become a complex number when | c o s a | > 1. It is noticed t h a t even if A ( l ) —> 0, cj> < (TT/8), or (37r/8) < just makes | c o s a | > 1. This makes a an imaginary number, which results the monotonic behavior of A(N), T(N), and R(N). For (n/8) < (f> < (3n/8), \cosa\ < 1; hence, a is mainly a real number with a small imaginary p a r t [A(l) 2ET (total energy), while Epoi is the correction introduced by polarization effects, which are however ignored in this case, regarding the motion of deuterons within the lattice. Charge density waves can also be calculated using the Hartree-Fock approximation. The simplest of these CDW states is obtained if it is assumed that all the electrons meet the same potential, independent of spin but periodic concerning their spatial position. This presupposition can be self-consistent and, under certain circumstances, the corresponding CDW state will have lower energy. The Coulomb energy contribution is greater in this case, but this increase is more than compensated for by the decrease in the energy of single particles of electrons just below the Fermi energy. This previous expression for quantum tunneling does not take account of the gradual variation with the distance r of the effective interaction between deuterons, or of the presence of any lattice impurities.

496

The aim of the present analysis is, instead, to study the effect of interaction between deuterons within a crystalline lattice on the process of cold fusion. Further, the lattices available for experimental investigation always contain a certain concentration of impurities, though small. Since one of the characteristic themes of our research has been the elaboration of a model which better reflects "real" processes, these two fundamental characteristics were accounted for by modifying the expression of the probability in order to establish whether they could contribute to the phenomenon by amplifying the tunneling effect, as previous studies 1 , 2 ' 3 indicated. With regard to the influence of impurities, it was found, for example, 3 that the probability of penetrating the Coulomb barrier increases on increasing the concentration of impurities. These appear to be able to concentrate in their vicinity a significant fraction of the deuterons present in the metal. The phenomenon shows characteristics analogous to the formation of a Cottrell 3 atmosphere in metals, known for some time in solid state physics. This essentially consists of a redistribution of the impurities present in the metal around a dislocation of the ions making up the lattice. In this case, the interaction between impurities and dislocations can significantly modify the electrical properties of the material. Further, particular reactions can occur, incorporating the impurities in the core of the dislocations as a result of the different arrangement of atoms with respect to that of the non-perturbed lattice. This type of process has been extensively studied in the literature in the case of high temperature crystalline semiconductors and metals. For the latter, it is demonstrated that the concentration of interstitial impurities around a linear dislocation with point component depends on the temperature according to a law of the type J = JQ exp((3/bkT), where Jo is the concentration of impurities in the zone with null internal pressure, o3 ~ Vi the volume of the ions making up the lattice, while (3 is proportional to the difference v

£ o c o a.

-50 J =0.75%

J =0.25%

-100

-150 0.1

0.2

0.3

0.4

0.5

0.6

0.7

/tA) Figure 1. In this figure a quantum model was used. The trends of the quantum potential (2), which contains the Morse contribution (3), (curve on left) and the modified semi-classical "shell" potential (7) (curve on right), are shown for different values of impurity concentrations. The dotted line (Lei) indicates the lowest energy level; the lower unbroken line indicates the total energy.

An interesting aspect, which merits further investigation, is the application these studies may have in a field completely different from the tunneling effect. Further theoretical and experimental studies are in course to analyze the non-semi-classical tunneling effect on human cells, to detect any mutations, tumor or otherwise, which may be induced. APPENDIX A The charge density in a CDW can be written as follows: (Al)

P = Po+ Pi cos[2fcFir +

(5)

(6)

506

and hence the total energy is 2

9

P

9

P

P

E = Ek + V = ^ - - - = ~ . (7) 2r r 2r Having r from Eq. (5) one can write the expression for the energy levels for hydrogen atoms

E==

(8)

-w^>

the same results were further obtained by quantum mechanics. Using the angular momentum quantization condition L = pr = nh/2w and Louis de Broglie's relationship p = h/\ between momentum and wavelength one can get 2irr = nX. (9) This means that the circular Bohr orbit is an integral number of the de Broglie wavelengths. The Bohr model is actually only accurate for a oneelectron system. 1.3. The Hydrogen

Atom

in Classical

Mechanics

Is it possible to understand some properties of a hydrogen atom from classical mechanics? The Hamiltonian for a hydrogen atom is

H = ^p- + ^--j^-r 2

2

\rp-fe\

(10) V

;

All notations are standard. The definition of the center of mass is mprp + mere = 0

(11)

and the relative distance between electron and proton is f=fp-re.

(12)

Equations (10)-(12) lead to the results: me r, re — p mp + me (ur2 2

mp mp + me''

e2 r '

(13)

(14)

where mpme

(15)

77ip + m e

The Hamiltonian (14) coincides with the Hamiltonian for the fictitious material point with reduced mass [i moving in the external field —e2/r. If we know the trajectory of this fictitious particle f = f(t), then we can reconstruct the trajectories of electron and proton using equations (13) r P (t) =

f ^ (t), mp + me

fe(t) =

^—f%t)mp + me

(16)

507

It is evident from (16) that the proton and electron move in the opposite directions synchronously. So the motions of proton, electron, and their relative motion occur with equal frequency (17) over the closed trajectories scaling by the ratio Ve_ _ mp v&_ _ m^ v-n me' v.. mR' xp

,ll,e

U^

llbe

vn

U-p

Vj^ _ mp m„

(18a)

//(.^

Schelaev4 proved that the frequency spectrum of any motion on ellipse contains only one harmonic. We can get from (16) that Pp = P,

Pe = -P,

(18b)

where — P\ = m\r\. All three impulses are equal to each other in absolute value, which means the equality of AD(p) = AD(e) = AD0*) = hAP-

(19)

Conclusion: Therefore, the motions of proton and electron and their relative motion occur with the same Frequency, Impulse (linear momentum) and the de Broglie wavelength. All motions are synchronized and self-sustained. Therefore, the whole system -hydrogen atom is nondecomposable to the independent motions of proton and electron despite the fact that the kinetic energy ratio of electron to proton is small:

# 4 4 = 4-46 xlCT4.

-Ek(p) This means that the nuclear and the corresponding atomic processes must be considered as a unified entirely determined whole process. For example, Weisskopf 5 came to the conclusion that the maximum height H of mountains in terms of the Bohr radius a is equal to -=2.6xl014, a and water wave lengths A on the surface of a lake in terms of the Bohr radius is equal to A 7 - « 2TT x 107. a Let us introduce the quantity / = rv, which is the invariant of motion, according to Kepler's second law, then \iv =

= —, r r and we can rewrite Eq. (14) in the following way: uf2 e2 U=M---. 2r2 r

(20)

(21) '

y

508

We can obtain the minimal value of (21) by taking its first derivative over r and setting it equal to zero. The minimal value occurs at M/

2

9

(22)

'

and the result is " m i n = -C'min =

—

e4 7;

~p^ •

(2o)

The values of invariant of motion vf (in MeV*s) can be calculate from (23) if we require the equality of Em\n to the energy of the ground state of a hydrogen atom fj,f = iivr = 6.582118 x 1(T 22 = h,

(24)

Conclusion: The Bohr quantization conditions were introduced as a hypothesis. We obtain these conditions from a classical Hamiltonian requiring its minimality. It should be strongly stressed that no assumption was formulated about trajectories of proton and electron. We reproduced exactly the Bohr result and modern quantum theory. The Plank constant h is the Erenfest adiabatic invariant for a hydrogen atom: \ivr = H. Let us briefly review our steps: • We used a well-established interaction between proton and electron. • We used a fundamental fact that the total energy = kinetic energy + potential energy. • We used Kepler's second law. • We used usual calculus to determine the minimum values of H. • We required the equality of Em[n to the energy of the ground state of hydrogen atom. Classical Hamiltonian + classical interaction between proton and electron + classical second Kepler law + standard variational calculus, together these well established steps in macrophysics reproduce exactly the results of microphysics; that is, the Bohr model and modern quantum theory (Schrodinger equation). We have not done anything spectacular or appealed to any revolutionary and breakthrough physics. Using the Newton equation with well-established interactions Gryzinski 6 proved that atoms have the quasicrystal structure with definite angles: 90°, 109°, and 120° which are the well-known angles in crystallography. 2. Nuclei and Atoms as Open Systems (1) LENR may be understood in terms of the known fundamental laws without any violation of basic physics. The fundamental laws of physics should be the same in micro- and macrosystems. (2) Weak and electromagnetic interactions may show a strong influence of the surrounding conditions on the nuclear processes.

509

(3) The conservation laws are valid for closed systems. Therefore, the failure of parity in weak interactions means that the corresponding systems are open systems. Periodic variations (24 h, 27, and 365 days in beta-decay rates indicate that the failure of parity in weak interactions has a cosmophysical origin. Modern quantum theory is the theory for closed systems. Therefore, it should be reformulated for open systems. The closed systems are idealization of nature, they do not exist in reality. (4) The universal resonance synchronization principle is a key issue to make a bridge between various scales of interactions and it is responsible for selforganization of hierarchical systems independent of substance, fields, and interactions. We give some arguments in favor of the mechanism - ORDER BASED on ORDER, declared by Schrodinger in Ref. 7, a fundamental problem of contemporary science. (5) The universal resonance synchronization principle became a fruitful interdisciplinary science of general laws of self-organized processes in different branches of physics, because it is the consequence of the energy conservation law and resonance character of any interaction between wave systems. We have proved the homology of the atom, molecule and crystal structures including living cells. Distances of these systems are commensurate with the de Broglie wavelength of an electron in the ground state of a hydrogen atom, it plays the role of the standard distance, for comparison. (6) First of all, the structure of a hydrogen atom should be established. A proton and electron in a hydrogen atom move with the same frequency that creates attractive forces between them; their motions are synchronized. A hydrogen atom represents the radiating and accepting antennas (dipole) interchanging energies with the surrounding substance. The sum of radiate and absorb energy flows by electron and proton in a stable orbit is equal to zero 8 - the secret of success of the Bohr model (nonradiation of the electron in a stable orbit). "The greatness of mountains, the finger sized drop, the shiver of a lake, and the smallness of an atom are all related by simple laws of nature." 5 (7) These flows create standing waves due to the resonance synchronization principle. A constant energy exchange with substances (with universes) create stable auto-oscillation systems in which the frequencies of external fields and all subsystems are commensurate. The relict radiation (the relict isotropic standing waves at T = 2.725 K - the Cosmic Microwave Background Radiation (CMBR)) and many isotropic standing waves in cosmic medium 9 should be results of self-organization of the stable hydrogen atoms, according to the universal resonance synchronization principle, that is a consequence of the fundamental energy conservation law. One of the fundamental predictions of the Hot Big Bang theory for the creation of the Universe is CMBR. (8) The cosmic isotropic standing waves (many of them are not discovered yet) should play the role of a conductor responsible for stability of elementary

510

particles, nuclei, atoms, . . . galaxies ranging in size more than 55 orders of magnitude. (9) The phase velocity of standing microwaves can be extremely high; therefore all objects of the Universe should get information from each other almost immediately using phase velocity. The aim of this paper is to discuss the possibility of inducing and controlling nuclear reactions at low temperatures and pressures by using different low-energy external fields and various physical and chemical processes. The main question is the following: is it possible to enhance LENR rates by using low and extremely low-energy external fields? The review of possible stimulation mechanisms is presented in Refs. 1 and 5. We will discuss new possible ways to enhance LENR rates in condensed matter. 3. LENR in Condensed Matter The modern understanding of the decay of the neutron is n —> p + e~ + ve.

(25)

The energetics of the decay can be analyzed using the concept of binding energy and the masses of particles by their rest mass energies. The energy balance from neutron decay can be calculated from the particle masses. The rest mass difference 0.7823 MeV/c 1 between neutron and (proton + electron) is converted to the kinetic energy of proton, electron and neutrino. The neutron is about 0.2% more massive than a proton, an energy difference is 1.29 MeV. A free neutron will decay with a half-life of about 10.3 min. Neutron in a nucleus will decay if a more stable nucleus results otherwise neutron in a nucleus will be stable. A half-life of neutron in nuclei changes dramatically and depends on the isotopes. The capture of electrons by protons is possible p + e~ —» n + z/e,

(26)

but for free protons and electrons this reaction has never been observed which is the case in nuclear + atomic physics. The capture of electrons by protons in a nucleus will occur if a more stable nucleus results. 3.1. Cooperative

Processes

The processes (25) and (26) in LENR occur with individual nucleons and electrons. In these cases the rest mass difference is equal to 0.7823 MeV/c . In the case of neutron decay the corresponding energy (Q = 0.7823 MeV) is converted to kinetic energies of proton, electron, and antineutrino. In the case of the capture of electrons by protons the quantity Q = 0.7823 MeV is a threshold electron kinetic energy under which the process (26) is forbidden for free proton and electron.

511

We have formulated the following postulate: The processes (25) and (26) in LENR occur in the whole system: cooperative processes including all nucleons in nuclei and electrons in atoms, in condensed matter. In these cases the threshold energy Q can be drastically decreased by internal energy of the whole system or even more - the electron capture by proton can be accompanied by emission of internal binding energy - main source of excess heat phenomenon in LENR. The processes (25) and (26) are weak processes. A weak interaction which is responsible for electron capture and other forms of beta decay is of a very short range. So the rate of electron capture and emission (internal conversion) is proportional to the density of electrons in nuclei. This means we can manage the electron-capture (emission) rate by the change of the total electron density in the nuclei using different low energy external fields. These fields can play the role of triggers for extracting the internal energy of the whole system or subsystems, changing quantum numbers of the initial states in such a way that forbidden transitions become allowed ones. The distances between proton and electron in atoms are of the order 10 ~6 — 10~5 cm and any external field decreasing these distances, even for a small value, can increase the process (26) in nuclei in an exponential way. Therefore, the influence of an external electron flux (discharge in condensed matter: breakdown, spark, and ark) on the velocity's processes (25) and (26) can be of great importance. The role of external electrons is the same as the catalytic role of neutrons in the case of the chain fission reactions in nuclei: neutrons bring to nuclei binding energies (about 8 MeV) which enhance the fission rates by about 30 orders. 4. Predicted Effects and Experimentum Cruices Postulated enhancement mechanism of LENR by external fields can be verified by the Exprimentum Cruices. We 8 predicted that natural geo-transmutation in the atmosphere and earth occur in the regions of a strong change in geo-, bio-, acousticand electromagnetic fields. The various electrodynamic processes at thunderstorms are responsible for different phenomena: electromagnetic pulses, 7-rays, electron fluxes, neutron fluxes, and radioactive nuclei fluxes. 4.1. Neutron

Production

by

Thunderstorms

The authors of Ref. f0 concluded that a neutron burst is associated with lighting. The total number of neutrons produced by one typical lighting discharge was estimated as 2.5 x 10 10 . 4.2. Production

of Radiocarbon

and Failing of Radiocarbon

Dating

The radiocarbon dating is based on the decay rate of radioactive isotope 14 C which is believed to be constant irrespective of the physical and chemical conditions.

512

The half-life of radiocarbon 14 C is 5730 years. A method for historical chronometry assuming was developed that the decay ratio of 14 C and its formation are constant in time. It was postulated that 14 C is formed only by the cosmic ray neutrons 14

N(n,p) 1 4 C.

(27a)

Radiocarbon dating is widely used in archeology, geology, antiquities,... There are over 130 radiocarbon dating laboratories. The radiocarbon method of dating was developed by Willard F. Libby who was awarded the Nobel prize in Chemistry for 1960. The radiocarbon method do is not take into account the following facts which have been established recently: • The neutron production by thunderstorms. 10 • The Production of radiocarbon by lighting bolts. 11 Let us consider the reaction 14

N + e - ^ 1 4 C + ^e,

(27b)

the Tfc(e) = 165.41 keV is the threshold energy which should by compared with 782.3keV for process (26). Production of radiocarbon by lighting bolts was established in Ref. 11. Unfortunately, this means FAILING of RADIOCARBON DATING. 4.3. Production

Radiophosphorus

by

Thunderstorms

The life-times of f§P and f|P are equal to 14.36 and 25.34 days, respectively. They were found in rain-water after thunderstorms. 12 Production of the radiophosphorus by thunderstorms can be understood in the following way: r6S + e-^ltP

+ ve,

(28)

fjjS + e - ^ P

+ i/e,

(29)

thresholds of these processes are equal to 1.710 and 0.240 MeV, respectively. The precipitation of MeV electrons from the inner radiation belt 13 and enhancement of the processes by lighting are possible. 4.4. LENR Stimulated

by Condensed

Matter

Discharge

Let us consider the condensed matter discharge (breakdown, spark, and arc) using the different electrodes. There are the following processes: (1) The electrode is Ni. Orbital or external electron capture iNi(68.27%) + e~ -> lfCo(70.78 days) + i/e.

(30)

The threshold Q\ = 0.37766 keV of this reaction on Ni should be compared with the threshold Qi = 0.7823 energy for electron capture by free protons:

513 Q2/Q1 ~ 2. The velocity of orbital electron capture can be enhanced by the discharge. (2) Orbital or external electron capture pCo(70.78 days) + e" -> ^Fe(0.28%) + ue,

(31)

with emission of energy Q2 = 2.30408 MeV. (3) Double orbital or external electron capture iNi(68.27%) + 2e" -> ^Fe(0.28%) + 2ue,

(32)

with emission of energy Qs = 1.92642 mostly by neutrinos. The proposed cooperative mechanism of LENR in this case can be proved in an extremely simple way: presence of radioactive 27C0 and enriched isotope of |gFe. This mechanism can give possibilities to get a way of controlling the necessary isotopes and excess heat. 4.5. Neutrinoless

Double Beta

Decay

1

As we know, the physical roles of electron and neutrino for LENR in condensed matter has not been investigated in detail up to now despite the fact that weak processes in nuclei are well understood. The double beta decay is the rarest spontaneous nuclear transition, in which the nuclear charge changes by two units while the mass number remains the same. Such a case can occur for the isobaric triplet A(Z,N), A(Z±l,N=fl), A(Z±2,NT%), in which the middle isobar has a greater rest mass than the extreme ones, and the extremes are the nuclei with the even Z and N. The usual beta-decay transferring a given nucleus into another via an intermediate nucleus is energetically forbidden. The double beta decay in nuclei can proceed in different modes: 14 • The two neutrino decay mode 2v(3j3 A(Z,N)

-> A(Z + 2,N-2)

+ 2e~+2ve)

(33)

which is allowed by the Standard Model of particle physics. The total kinetic energy of two emitted electrons present continuous spectra up to £ m a x . • The neutrinoless mode Ov/3/3 A(Z, N) -> A(Z + 2, N - 2) + 2e",

(34)

which requires violation of a lepton number. The total kinetic energy of two emitted electrons is equal to Emax. Two neutrinos in the mode 2v(3/3 carry out almost all emitted energies, which is useless for practical applications; therefore, this mode is not important for us. A fundamental question is: does the neutrinoless double beta decay exist or not (for the review of the history see Ref. 14). The emerged energies in the neutrinoless 0^/3/3 mode are easily detected for practical use but these are the rarest spontaneous nuclear transitions (T « 10 18 - 1030 years). Is it possible to enhance the decay rate?

514

Above and in Refs. 1-3, we have discussed the cooperative and resonance synchronization enhancement mechanisms of LENR. Some of the low energy external fields can be used as triggers for starting and enhancing of exothermic LENR. It is natural to expect that in the case of beta-decay (capture) the external electron flux with high density, or a laser of high intensity, or any suitable external fields should play this role. Any external field shortening distances between protons in nuclei and electrons in atoms should enhance beta-decay (capture) or double-beta decay (capture). There are a great number of experiments in Japan, Italy, Russia, US, India, China, Israel, and Canada in which cold transmutations and excess energy were measured (see http://www.lenr-canr.org). It is very popular to use Ni, Pd, Pt, and W as electrodes in the condensed matter discharge (breakdown, spark, arc, and explosion) experiments. Let us consider the case Pd electrodes. The difference of the rest mass of m Qe°Pd) - m Q|°Cd) = 1.9989 MeV/c 2 , therefore, the external field can open the channel 46°Pd —> 4g°Cd with Q = 1.9989. The experimental data 1 5 seem to confirm such expectations. Therefore, expensive and time-consuming double beta decay experiments can be performed in cheap and short-time experiments by using suitable external fields. This direction of research can open production of new elements (utilization of radioactive waste) and excess heat without of ecological problem. A careful analysis of the double beta decay shows that the 2e~ cluster can be responsible for the double beta decay. The difference between the rest mass 56°Ba and 52°Te, which is equal to 92.55 keV, indicates the possibilities to capture the 4e~ cluster by j ^ B a . It is a full analogy with the Iwamura reactions. 16 The lack of financial support and the ignorance from the whole physical society of LENR lead to catastrophes. The mechanism of shortening the runaway of the reactor at the Chernobyl Nuclear Power Plant and catastrophes induced by the High Frequency Active Auroral Research Program (HAARP) program is based on our postulated cooperative resonance synchronization mechanism. The same mechanism should be responsible for the International Experimental Fusion Reactor (ITER) explosion in future.

5. Conclusion We proposed a new mechanism of LENR: cooperative processes in whole the system - nuclei + atoms + condensed matter can occur at a smaller threshold energies than the corresponding ones on free constituents. The cooperative processes can be induced and enhanced by low energy external fields. The excess heat is the emission of internal energy and transmutations at LENR are the result of redistribution of inner energy of the whole system.

515

References 1. F.A. Gareev, I.E. Zhidkova, and Yu.L. Ratis, Preprint JINR P4-2004-68, Dubna, 2004 (in Russian); in: Proceedings of the 11-th Russian Conference on Cold Nuclear Transmutation of Chemical Elements and Ball Lighting, Dagomys, city Sochi, September 28 - October 5, 2003, Moscow 2004, p. 169. 2. F.A. Gareev, in: FPB-98, Novosibirsk, June 1998, p. 92; F.A. Gareev, G.F. Gareeva, in: Novosibirsk, July 2000, p. 161. 3. F.A Gareev, I.E. Zhidkova, and Yu.L. Ratis, in Program Abstracts on ICCF-11, Marseille: France: 2004, 31 October - 5 November; F.A. Gareev, I.E. Zhidkova, E-print arXiv Nucl-th/0505021 vl 8 May 2005; E-print arXiv nucl-th/0511092, Vol. I, 30 November 2005. 4. LA. Schelaev, FPV-2004 (Novosibirsk, 2004), Vol. II, p. 27. 5. V.F. Weisskopf, Am. J. Phys. 54 (2), 110 (1986). 6. M. Gryzinski, FPV-2004, Vol. I (Novosibirsk, 2004). 7. E. Schrodinger, What is Life? The Physical Aspects of the Living Cell (Cambridge University Press, Cambridge, 1967). 8. F.A. Gareev, I.E. Zhidkova, and Yu.L. Ratis, Appl. Phys. J. N 3 , 25 (2005). http://www.iscmns.org/siena05/program.htm. 9. A.M. Chechelnitsky, E-print arXiv: physics/0105056 (2001). 10. L.S. Bratolyubova-Tsulukidze et al, Adv. Space Res. 34, 1815 (2004). 11. L.M. Libby and H.R. Luken, J. Geophys. Res. 78, 5902 (1973). 12. LP. Selinov, Isotops (Nauka, Moscow, 1970). 13. U.S. Unan et al, Geophys. Res. Lett. 15, 172 (1988). 14. H.V. Klapdor-Kleingrothaus and A. Staudt, Teilchenphysik Ohne Besschleuniger (B.G.Teubner, Stutgart, 1995). 15. LB. Savvatimova and A.D. Senchukov, ICCF6 2, 575 (1996). 16. Y. Iwamura, ICCF11 (2005). 17. O.R. Grogoryan, A.V. Sinyakov, and S.I. Klimov, Adv. Space Res. 20, 389 (1997). 18. L.S. Bratolyubova-Tsulukidze et al., Cosmic Res. 39, 602 (2001).

P O L Y N E U T R O N THEORY OF T R A N S M U T A T I O N

J O H N C. F I S H E R 600 Arbol Verde, Carpinteria, CA 93013, E-mail: [email protected]

USA

Polyneutron theory is applied to nuclear transmutation. Implications of the theory are compared with experiment. Additional more definitive experiments are suggested.

Polyneutron theory postulates that large clusters of neutrons are bound and stable against strong decay and that their interactions with ordinary nuclei are responsible for a new class of low-temperature nuclear phenomena. It is postulated that these clusters, also termed polyneutrons or neutron isotopes, grow to include hundreds of neutrons in chain reactions fueled by isotopes such as 2 H, 1 8 0 , and 7 Li. 1 It is anticipated that an ordinary nucleus AX and a polyneutron B n can bind to form a composite AXBn that subsequently decays by transfers or exchanges of nucleons between its components. The present analysis focuses on composite formation and on the transmutations that result from composite decay. I assume that the neutrons in polyneutrons are paired with the BCS symmetry first described for electrons in superconductors, 2 and that breaking a pair requires so much energy that odd-numbered polyneutrons can be produced only in reaction with deuterium. In the reaction 2An + 2 H —> 2A+1n + 1 H transmutation of H makes available up to 5.847 MeV for adding the odd neutron. If the mass excess of 2A+1n were to exceed that of 2An by (say) 5 MeV, the reaction forming it would be exothermic by 0.847 MeV. On the other hand the reaction 2 A + 1 n + 2 H -> 2A+2n + *H would be exothermic by 10.847 MeV with a much larger cross section, and in a chain reaction where polyneutrons are growing and fissioning in interaction with 2 H, as in the experiments of Iwamura et al.,3~5 the concentration of even polyneutrons is expected to substantially exceed that of odd ones. Hence as a first approximation I consider only even polyneutrons. Transmutations associated with composite formation and decay are expected to occur at differing rates. Formation is expected to be the limiting rate, depending as it does on the very small concentration of polyneutrons. Strong reactions that do not require associated beta decay or electron capture are assumed to be most rapid, and to occur during composite formation. Weak reactions that require associated beta decay or electron capture are assumed to be slower. Weak reactions that require associated double beta decay or double electron capture are assumed to be slower still, followed by reactions that require three or more associated weak 516

517

reactions. With the foregoing assumptions the following procedure determines the sequence of transmutations according to the present status of the theory: Step 1. Consider a starting element G X for which we desire to know the isotopes to which it may be transmuted by interaction with polyneutrons. The first step is formation of a composite ^X B n in a reaction such as ^X + D n —> ^X B n + G+D_yl B ^ n . Such a reaction can only occur in an environment where polyneutrons are continuously being created, as in the active region of an ongoing chain reaction. In a newly formed composite the value of A is that for which the composite is stable against the strong reactions ^X B n —> A+1^.XB~Nn for all positive and negative even values of N. These reactions must be endothermic. The energy they release is EQ = A(-^X) — /S.(A+NZX) + NS, where S represents half the change in polyneutron mass excess associated with adding a pair of neutrons, 5 = (l/2)[A( j 4 + 2 n) —A(' 4 n)]. The reaction is exothermic for EQ > 0. Are any such transfers exothermic? If yes, choose the most exothermic among N = ±2, ±4, ± 6 , . . . , and go to Step 2. If no, go directly to Step 2. Step 2. Represent the output of the previous step by ^X. Is there an isotope zi'i'Y of the element having one more or one less proton than AX that can be reached by exchange or transfer of nucleons within the composite? (Each of these reactions requires an associated beta decay or electron capture.) The energy released is Ei = A(^X) —A( J±(Y) + N5. Are any such transfers exothermic? If yes, choose the most exothermic among z = ± 1 and N = 0, ±2, ± 4 , . . . , and return to Step 2. If no, go to Step 3. Step 3. Represent the output of the previous step by AX. Is there an isotope A ^±2^ of the element having two more or two fewer protons than AX that can be reached by exchange or transfer of nucleons within the composite? (Each of these transfers requires two associated beta decays or electron captures.) The energy released is E^ = A(AX) — A( 0"±2Y) + NS. Are any such transfers exothermic? If yes, choose the most exothermic among z ± 1 and N = 0, ±2, ± 4 , . . . , and go to Step 2. If no, continue with three or more associated weak decays, or stop if transmutations with such decays are neglected. The beta decays in Steps 2 and 3 can be imagined as occurring in the polyneutron in association with transfer of the resulting proton to the ordinary nucleus. For N = 0 each proton so formed exchanges with a neutron from the ordinary nucleus, accelerating the rate of N = 0 beta decays to match that of N ^ 0 decays. Electron captures can be imagined as occurring in association with transfer of a proton from the ordinary nucleus to the polyneutron. For N = 0 each proton so transferred exchanges with a neutron from the polyneutron, accelerating the rate of N = 0 electron captures to match that of N ^ 0 captures. Examples of reactions and their energies are shown here in more detail. No beta decay:

fXBn^A+NzXB~Nn E0 = A(AX)

- A(A+N2X)

+ E0, + N5.

518

Single beta decay:

Single electron capture: ^ n ^ ^ Y ^ n Ex = A(AX)

+ i^,

- A( A z t?Y) + N6.

Double beta decay: *XBn^Az++N2YB-Nn E2 = A(AX)

- A(A\N2Y)

+ E2, + N5.

Double electron capture: ^ X B n ^ A z t ^ Y B " i v n + £;2,

E2 = A{AX) - A ( ^ Y ) + NS. In my calculations, I assume that 5 is independent of A with the value S = 1.143 as tentatively determined from transmutation of 138 Ba to 150 Sm. With this value of 5, and assuming that the binding energy of a composite is independent of the properties of its components, it is possible to calculate the transmutation chain for any starting isotope. (The assumption of constant 5 holds only approximately over a limited range of values of A, and the assumption of a constant binding energy for composites ignores the influence of shell structure of the ordinary nucleus and of the sizes of both components. These questions should be addressed in a more realistic treatment of the theory.) Transmutation chains can be more easily visualized by simplifying the notation. Abbreviate the composite AX n as (^X) where the size of the polyneutron component is understood. Then as an example the transmutation 139 La n —> 141 Ce ~~ n is abbreviated ( 139 La) —> ( 141 Ce). With this notation, and neglecting transmutations with three or more associated weak interactions, the transmutation chain for 139 La is 139

La + An -+ ( 139 La) - ( 141 Ce) -+ ( 141 Pr) -

( 143 Nd).

In addition to these decay channels, each composite has a side channel that frees the ordinary nucleus and substitutes a helium nucleus, typified by 141

CeAn^4HeA~4n +

141

Ce.

In consequence, accompanying the composite decay chain there is in its wake a residual of free isotopes 141 Ce, 141 Pr, 143 Nb whose numbers depend on the relative magnitudes of the side channels. To recapitulate, I assume that formation of the initial composite ( 139 La) is the rate-limiting step. Once a composite has formed, I assume that it decays rapidly through the chain leaving behind a residue of free

519

transmuted isotopes that can be revealed by mass spectrometry. Shortly after composite formation ceases, signals for 139 La, 141 Ce, 141 Pr, and 143 Nb would be revealed; perhaps with the largest signal for 143 Nb if the side reactions are small and most composites survive to the end, or perhaps with the smallest signal if the side reactions are larger and deplete the composites as they pass through successive transmutations. At a later time after composite formation ceases mass spectrometry would detect signals only for 139 La, 141 Pr, and 143 Nb with an enhanced 1 4 1 Pr signal from beta decay of 141 Ce with its 33 day half life. I now consider the transmutations investigated by Iwamura et al.3~5 Transmutation of 138 Ba is reported to lead to 150 Sm. The decay chain predicted by polyneutron theory is 138Ba

+

An _+ ( 1 3 8 B a ) _> ( 1 4 0 C e ) _> ( 1 4 4 N d ) _>

(150gm)

^

(

158Gd)

leaving residual amounts of 140 Ce, 144 Nd, 150 Sm, 158 Gd, and so on. It leaves a residue of free 150 Sm nuclei only for values of S that lie in the narrow range 1.142 < S < 1.144. This is the basis for my assumption that S = 1.143. Transmutation of 88 Sr is reported to lead to 96 Mo. The reaction chain predicted by the theory is 88

Sr + An -+ ( 90 Sr) -> ( 92 Y) -+ ( 96 Zr) ^ ( 96 Nb) ^ ( 100 Mo) -+ ( 102 Tc) ^ • • •

leaving residual amounts of 90 Sr, 92 Y, 96 Zr, 96 Nb, 100 Mo, 102 Tc, and so on. The 96 Nb residue decays to 96 Mo with a half life of 23 h. During composite formation, mass spectrometry will reveal a signal at mass 96 from residual 96 Zr and 96 Nb, along with 96 Mo from decay of 96 Nb. A few days after composite formation has ceased the mass signal will come from 96 Zr and 96 Mo with an enhanced 96 Mo component from decay of 96 Nb. A Mo signal from XPS will be obtained from the 96 Mo and 100 Mo residuals. Transmutation of 133 Cs is reported to lead to 141 Pr, and to as yet unidentified isotopes with intermediate masses between 133 and 141. The theory predicts 133

Cs+A

n - ( 137 Cs) -+ ( 137 Ba) - ( 139 La) - ( 141 Ce) -+ ( 141 Pr) ^ ( 143 Nd)

leaving residual amounts of 137 Cs, 137 Ba, 139 La, 141 Ce, 141 Pr, and 143 Nd. The latter portion of this chain was treated in the example above for transmutation of 139 La, in which a signal for 1 4 1 Pr arose from the 1 4 1 Pr residual plus additional 141 Pr from decay of 141 Ce. Finally transmutation of 137 Ba was reported to lead to a signal at mass 149, tentatively attributed to 149 Sm although no XPS signal for Sm could be detected. Theory predicts the decay chain 137Ba

+

An_^

(137Ba)

^

(139La)

^

(141Ce)

^

(141pr)

^

(

143Nd)

leaving residual amounts of 139 La, 141 Ce, 141 Pr, and 143 Nd as for transmutation of 133 Cs. No signal for Sm is expected. (It may be that the reported mass 149 signal represents 137 Ba 12 C or 1 3 3 Cs 1 6 0 from contamination by carbon or cesium during the transmutation process.)

520 Overall the agreement between theory and the experiments of Iwamura et al. is suggestive but not definitive. Consideration of other t r a n s m u t a t i o n chains identifies experiments t h a t could be more definitive. T h e parameter choice 5 = 1.143 implies t h a t 2 0 7 P b and 2 0 8 P b are absolutely stable, all potential t r a n s m u t a t i o n s involving any number of possible associated weak interactions being endothermic. Looked at another way, these P b isotopes are the final products of t r a n s m u t a t i o n of every starting element, provided only t h a t sufficient time is allowed. Nuclei lighter t h a n lead t r a n s m u t e by b e t a decay alone, as in 205 T 1 +

An^(205T1)^(207pb)>

Nuclei heavier t h a n lead t r a n s m u t e by electron capture alone, as in 209

Bi + ^ n ^ ( 2 0 9 B i ) ^ ( 2 0 7 P b ) .

Lead isotopes 2 0 4 P b and 2 0 6 P b t r a n s m u t e by neutron transfer in association with composite formation, as in 204

Pb+

A

206

Pb+

A

n^ n^

(208Pb), (208Pb).

These transmutations are ideal testing grounds for the theory. T h e y suggest t h a t polyneutrons can induce transmutations where the final nucleus differs from the starting nucleus by addition of a proton and a neutron, by subtraction of a proton and a neutron, or by addition of two or four neutrons. Each of these reactions requires only a single step from composite formation to the final 2 0 7 P b or 2 0 8 P b product. Because the product is stable, one-to-one substitution of 2 0 7 P b for 2 0 5 T1 and for 2 0 9 Bi should be seen, as should substitution of 2 0 8 P b for 2 0 4 P b and 2 0 6 P b . T h e predictions of the theory are definite and clear-cut, although minor corrections can be expected when the analysis is extended to include odd polyneutrons. If the predictions are borne out by experiment the credibility of the theory will be enhanced. If not the theory will face a crisis.

References 1. 2. 3. 4.

J. C. Fisher, Fusion Tech. 34, 66 (1998). J. Bardeen, L. N. Cooper, and J. R. Schrieffer, Phys. Rev. 108, 1175 (1957). Y. Iwamura, M. Sakano, and T. Itoh, Jpn. J. Appl. Phys., 4 1 , 4642 (2002). Y. Iwamura, T. Itoh, M. Sakano, N. Yamazaki, S. Kuribayashi, Y. Terada, T. Ishikawa, and J. Kasagi, Proc. ICCF 11 (World Scientific Inc., 2006), 339. 5. Y. Iwamura, T. Itoh, M. Sakano, N. Yamazaki, S. Kuribayashi, Y. Terada, and T. Ishikawa, Proc. ICCF 12 (World Scientific Inc., 2006), to be published.

T H E T H E R M A L C O N D U C T I O N FROM THE C E N T E R S OF T H E N U C L E A R R E A C T I O N S IN SOLIDS

KEN-ICHI TSUCHIYA Department of Chemical Science and Engineering, Tokyo National College of Technology, 1220-2 Kunugida, Hachioji, Tokyo 193-0997, Japan E-mail: [email protected]

If nuclear reactions happen in solids, heat generated from the reaction center is diffused. In this study, the thermal conduction from the centers of a DD reaction in solids induced by the Bose—Einstein condensation is considered. The voids in solids are assumed as the sites of the reaction centers. The equations of the thermal conduction are solved using Fourier expansion. The calculated results show the rapid temperature relaxation. This means that nuclear reactions in solids do not induce thermal explosions.

1. D D Reaction Rate in Solid In the previous work,1 DD reaction rate in Pd void is calculated applying the equivalent linear two-body (ELTB) method. The rate is determined by the ELTB ground state wave function ^> for N identical charged Bose nuclei as

R=

m¥)—'

(1)

where imaginary part of Fermi pseudopotential V? 2 ' 3 is written as ImV£

Ah = -—Sin-rj).

(2)

The short-range interactions of nuclear forces between two Bose nuclei are introduced by using 6 function. 2 ' 3 The constant A is given by the Bohr radius TB and the S factor of the nuclear reaction between two nuclei as A = 2Sr-e,/-Kh. The ELTB solution also gives the critical temperature Tc of Bose-Einstein condensation (BEC) by well-known formula which is written as h2

(

n

\2/3

where n is the local number density of Bose particles and (,{Z) is the Riemann's zeta function. The probability of the ground-state occupation is given by / ji \

2

/3

f2 = 1 - f - J

forT Tc, no nuclear reactions happen because fi = 0. The trapped site for a deuteron cluster is shown in Fig. 1. The calculated results for Tc and R are listed in Table 1. When N > 4 with using nonlinear screening, 4,5 Tc is higher than the room temperature. The ELTB solution is plotted in Fig. 2 for the case of the 5-deuteron cluster trapped at VacO.

Figure 1. The structure of VacO in fee lattice. The black and the gray circles mean occupied and unoccupied lattice points, respectively. These defects construct octahedral void, which is called VacO in this paper. Table 1. The nuclear reaction rate R(10 7 s _ 1 ) and the critical temperature T C (K) for the case of N deuterons rapped at VacO in Pd Nonlinear screening

Thomas- Fermi screening TV

Tc

R

Tc

R

3 4 5 6 7

56 66 76 86 95

2.1 3.5 5.0 6.7 8.6

257 329 403 480 558

33.8 66.4 108.6 160.2 221.3

2. Thermal Conduction If nuclear reactions happen in solids, heat generated from the reaction center is diffused. In this study, the thermal conduction from the center of a DD reaction in Pd is estimated. The equation of the thermal conduction in solid is written as dT

~m

fcV2T,

(5)

where T is the deviation of the temperature from the equivalent value and t is the time from a reaction. The constant k is defined as k=

K/Cp,

(6)

where constants K, C, and p mean the thermal conductivity (75.5 J / s m K ) , the specific heat (25 J/mol K) and the density (12.0 g/cm 3 = 12.0 x 10 6 /166.4mol/m 3 ),

523

;

1

! p/x 2

1I

£

i2

i

i


^i) ordinates alone.

ip5 d TV

•d 3 r 4 ,

(6)

12 an

d ^5

=

V'sC^ii • • •

I^A)

are

functions of spatial co-

532

5. T r a n s i t i o n M a t r i x E l e m e n t for a T — 0 F u s i o n R e a c t i o n We can now formally calculate the reaction matrix elements for the d - d fusion reactions including phonon coupling. Since we are focusing on isospin-preserving T = 0 matrix elements, this calculation applies to isospin-preserving reaction models. T h e relevant states are: • One 4 + 0 state of 4 He in a spin singlet ground state (mostly spatially symmetric). • One 2 + 2 state of two deuterons in a quintet spin 2 state. a • Two 3 + 1 states (since these can be singlets or triplets). These are a linear superpositions of the H + p and He + n states.

5 . 1 . Physical

Wavefunctions

T h e wavefunctions discussed above are formal R S T objects, which are very general. We need to focus on specific wavefunctions for the different mass 4 (T = 0) channels in order to proceed. For example, the wavefunction for the ground state 4 He nucleus can be taken to be just \l/i with a spatial p a r t t h a t is completely symmetric. Hence #4,0

=

1plO—f=[s5t6-S6t5].

(7)

For simplicity, we adopt a wavefunction for two deuterons t h a t are in a quintet (spin 2) state. In this case, we can use #2,2 = A{^(12;34:)swt6}.

(8)

Here, A is an antisymmetrizer, and ^ ( 1 2 ; 34) is the spatial part of the deuteron wavefunctions. This wavefunction can be taken to be of the form V(12; 34) = Mr2

- r i ) 0 d ( r 4 - ?3) F ( j

1

^ ,

^ ± ^ j

.

(9)

There are two kinds of 3 + 1 wavefunctions, including singlet and triplet states. T h e singlet S = 0 states can be written a s b #3,1 = ^ J V ( 1 2 3 ; 4 ) | ( s 5 t i 2 i ( m T = l / 2 ) U -s&t211(mT

• ^ ( 1 2 3 ; 4 ) i ( s 5 i i 2 i ( m T = - l / 2 ) U -s6t211{mT

= l/2)

U)

=-1/2)

|4) } . (10)

a

We should, in general, consider the deuterons to be in a singlet or triplet as well. However, we are only doing an example here. In this enumeration of states, we are ignoring the various Mg values. The subscripts 211, 121, and 111 are the Yamanouchi symbols for the 3-body wavefunctions

533

The 3+1 triplet S = 1 states can be written as %A = X | 0 ( 1 2 3 ; 4 ) i ( s 8 t i 2 1 ( m T = 1/2) U ~sQt2ll{mT

= l/2) j 4 )

-V(123;4)^(s 8 ti2i(mT = - l / 2 ) T 4 - S 9 t 2 i i ( m T = - l / 2 ) T 4 ) ] . (11) We used the notation | 4 or J.4 to refer to the isospin of the fourth particle. The spatial part of ^ i and ^'3 1 is of the form ^(123; 4) = 0 3 (ri, r2, r 3 ) F> (Vl

+

^

+

^ , r4) ,

(12)

where 03 only depends on the two co-ordinate differences such as f\ —ri and r^ — r^. 5.2. Physical

Wavej"unctions

in Terms of Ladder Basis

States

To compute the matrix element, we need to change basis and describe our physical wavefunctions in terms of our ladder basis. This change of basis can be accomplished either using induction coefficients of the symmetric group or by brute force calculations. The results are c •4{*4,o} = * i ,

-4{* 2 , 2 } = * 6 -

(13)

The definition of the ladder basis i state involves the fully symmetric tpio spatial wavefunction, which is well defined for the 4 He nucleus. In the case of two deuteron states, the ladder basis \&6 is expressed in terms of mixed symmetry spatial wavefunctions %p5 and -06- For the physical state we used, these mixed symmetry spatial wavefunctions can be written as 0 5 = - L [2^(12; 34) + 2^(34; 21) - 0(23; 14) - ^(14; 23) - 0>(13; 24) - (24; 13)], V 12

4>s = \ [-^(23; 14) - ^(14; 23) + 0,(13; 24) + 0(24; 13)]. In the case of the singlet 3+1 channel, the antisymmetrizer acts to produce a single ladder basis state *4{*3,i} = * i ,

(14)

where the associated fully symmetric spatial part -0io can be expressed as a symmetric combination of the physical 3+1 states as ^10 = \ [0(123; 4) + 0(124; 3) +^(134; 2) +0,(234;!)]. c

(15)

T h e results will only involve * i , \&4, and \&6- These wavefunctions and no others are involved because of group theoretical considerations and our assumptions that the spatial part of the deuteron, triton, and helium wavefunctions are symmetric under the exchange of any two particles.

534

In the case of the triplet 3+1 channel, the antisymmetrizer acts to produce a single ladder basis state A{*'3il}

= *4)

(16)

where the associated mixed symmetry spatial parts I^T, ip$, and xpg are V>7 = ^ L [3^(123; 4) - ^(124; 3) - ^(134; 2) - V(234; 1)],

(17)

V 12

^ 8 = - ^ [4^(124; 3) - V(134; 2) - ^(234; 1)],

(18)

V9 = - ^ ( 1 3 4 ; 2 ) - V ( 2 3 4 ; l ) ] .

(19)

The computation of the relevant matrix elements is made simpler because we have a complete set of results for the matrix elements available in terms of the ladder basis. 6. Matrix Elements We focus here on one specific example: ( ^ { * 3 , i ( M s = 0 ) } | y T | ^ { * 2 , 2 ( M s = l)}) =

(*i(M 8 =0)|V r |*6(M 1 , = l)).

(20)

The rest of the matrix elements can be calculated similarly. From our previous example we know that

=

/

/'

^1*0

3 ^ (a 12 + iyu) Z12 ypjrn) r 12

^ d

f\ • • • d

?4.

We can use this with the appropriate definitions of the spatial wavefunctions for the different channels: •05 = ~4= [2^(12; 34) + 2V>(34; 21) - ^(23; 14) - ^(14; 23) - V(13; 24) - ip(24; 13)] , V 12

(21) V-io = \ [V>(123; 4) + V(124; 3) + ^(134; 2) + ^(234; 1)].

(22)

7. Conclusions To include phonon exchange in a description of nuclear reactions, we require a description explicitly in terms of spatial wavefunctions. We have developed a complete set of such nuclear wavefunctions for the 2-body, 3-body, and 4-body problems using a ladder basis. Results for the 4-body case is presented above. A complete set of matrix elements for the HJ potential has been developed in terms of explicit spatial integrals. Antisymmetric wavefunctions that are appropriate for d-d fusion calculations in the T = 0 approximation have been developed, and we have presented a specific example in this paper.

535

Acknowledgments Support for I. C h a u d h a r y was provided by the Kimmel Fund, Bose Foundation, and from a D a r p a subcontract.

References 1. M. Hamermesh, Group Theory and its Applications to Physical Problems (AddisonWesley, New York, 1962). 2. T. Hamada and I.D. Johnston, Nucl. Phys. A34, 382 (1962).

S T U D Y ON FORMATION OF T E T R A H E D R A L OR OCTAHEDRAL S Y M M E T R I C C O N D E N S A T I O N B Y H O P P I N G OF ALKALI OR ALKALINE-EARTH METAL ION

HIDEMI MIURA 1-27-6 Tsurugaoka, Izumi-ku, Sendai 981-3109, E-mail: miubrewer@h9. dion. ne.jp

Japan

Formation of tetrahedral or octahedral condensation related to the experiments on electrolysis or deuterium permeation was studied. We obtained the scenario about the formation that alkali or alkaline-earth metal ions infiltrating into the host metal made cavities there when they hopped onto the other sites of the crystal lattice of it, then through squeezing of H + / D + ions in the cavity tetrahedral or octahedral condensation of protons/deuterons is caused.

1. Introduction Much research on nuclear fusion and nuclear transmutation in condensed matter is currently in progress. Recently, experiments with deuterium permeation through Pd complex by Iwamura et al. have indicated that nuclear transmutations occur with alternating CaO and Pd layers, but no nuclear reaction is observed when this material is replacing it with MgO. 1 On the theoretical side, we have directed our attention to Tetrahedral Symmetric Condensate/Octahedral Symmetric Condensate (TSC/OSC) model of protons/deuterons by Takahashi, which can explain consistently the major experimental results. 2 " 4 We have examined the role of the alkali and alkaline-earth metal ions in the crystal lattice of the host metal when TSC/OSC is formed. As a result, we have obtained a very consistent and simple scenario as one of hypotheses about the formation of TSC/OSC that the alkali or alkaline-earth metal ions infiltrating into the host metal make cavities there, when they hop onto the other sites of the crystal lattice, then through squeezing of H+/D+ ions in the cavity the protons or deuterons undergo TSC/OSC. 2. Scenario of Formation of T S C / O S C Experiments on nuclear fusion and nuclear transmutation in condensed matter are performed, for example, by the electrolysis of LiOH/LiOD or K2CO electrolytic solution using Ni or Pd cathode, and by the deuterium permeation through alternating CaO and Pd layers, respectively. The scenario about the formation of TSC/OSC is constructed from following five processes that would proceed in the face-centered cubic (fee) lattice of the hydride-forming metals. This scenario would be as simple as possible with the role of the alkali or alkaline-earth metal ions. 536

537

2.1. Permeation

of H+/D+

Ions

Figure 1 shows the permeation of H+/D+ ions and typical infiltration of alkali or alkaline-earth metal ions in the case of electrolysis of water and in a deuterium permeation experiment. Electrolysys

Deuterium permeation

Tetrahedron

Octahedron

Q:Ni/Pd

Figure 1. (typical).

D:Tsite

O : 0 site

Permeation of H + / D + ions and Infiltration of alkali or alkaline-earth metal ions

H+/D+ ions permeate into the fee crystal lattice of the host metal such as Ni and Pd by electrolytic voltage and D2 gas pressure, and they are located mostly at the O sites. Although H+/D+ ions move corresponding to the permeation rates, they are confined at the O sites of the crystal lattice of the host metal for a short while. 2.2. Infiltration

of Alkali or Alkaline-earth +

Metal

Ions

Alkali metal ions such as Li and K and alkaline-earth metal ions such as Ca 2 + infiltrate into the fee crystal lattice of it, and they come to the T sites, O sites, and the lattice voids or defects. In the case of electrolysis, alkali metal ions accumulating on the surface of the host metal infiltrate into the near surface layers due to the surface vibration and the electrolytic current, and then mostly stay at the T sites of the crystal lattice for a long while. Each of the alkali metal ions at the T sites vibrating thermally interacts with four H + / D + ions at the vertexes of the tetrahedron surrounding it and vibrates them widely. In the case of deuterium permeation, alkaline-earth metal ions staying in contact with the surface of the host metal also infiltrate into it due to the surface vibration and the deuterium flow, and then mostly stay at the lattice voids or defects for a long while. Each of the alkaline-earth metal ions at the lattice void or defect vibrating thermally also interacts with six H+/D+ ions at the vertexes of the octahedron surrounding it and vibrates them widely. 2.3. Hopping

+

of Alkali or Alkaline-earth

Metal

Ions

Figure 2 shows typical case of hopping of alkali or alkaline-earth metal ions, squeezing of H + / D + ions, recoil and condensation of protons/deuterons. The alkali metal

538

ions hop onto the other sites of the crystal lattice of the host metal due to the thermal vibration, electrolytic voltage and most probably some electromagnetic impulses, and then make cavities at the former positions. The alkaline-earth metal ions also hop due to thermal vibration, deuterium flux, and electromagnetic impulses, also making cavities.

Impulse

fi#o " 4p/TSC, 4dfTSC

V Condensed and recoiled * S • i f / K+ V ^ Tetrahedron 4^:Ca + O^Ni/Pd

D:Tsite

V Condensed and recoiled 6d/0SC Octahedron O : o site

Figure 2. Hopping of alkali or alkaline-earth metal ions, Squeezing of H + / D ions, Recoil and Condensation of protons/deuterons (typical).

2.4. Squeezing

of H+/D+

Ions and Recoil

The hopping of the alkali or alkaline-earth metal ion causes the cooling down of the cavity and the recoil of cluster H + / D + ions around it. The cluster H + / D + ions, namely protons/deuterons at the vertexes of the tetrahedron or octahedron that make up the surface of the cavity, are squeezed in the center of each polyhedron due to the reaction of hopping-out of the alkali or alkaline-earth metal ion. A heavy alkali or alkaline-earth metal ion causes the strong recoil of even heavy cluster H + / D + ions, while a light alkali or alkaline-earth metal ion causes the weak recoil of only light cluster H + / D + ions. 2.5. Condensation Transmutation

of Protons/Deuterons or Fusion

and

Nuclear

In the combination of strong recoil of squeezed cluster H + / D + ions, after the condensation of protons/deuterons, condensed 4p/TSC, 4d/TSC or 6d/OSC would collide against the atomic nucleus of the crystal lattice of the host metal or other one to cause the nuclear absorption and transmutation according to the Takahashi's TSC/OSC nuclear absorption theory 2 ~ 4 . In the case of 4p/TSC by Li or K in the T site of Ni: 4p/TSC + M(A, Z) -»• M*(A + 4, Z + 4), others.

(1)

In the case of 4d/TSC by K or Ca in the T site of Pd: 4d/TSC + M(A, Z) -> M*{A + 8, Z + 4), others.

(2)

539

In the case of 6d/OSC by Ca in the lattice defect or void of Pd: 6d/OSC + M(A, Z) -> M*(A + 12, Z + 6), others.

(3)

On the other hand, in the combination of weak recoil of squeezed cluster H+/D+ ions, after the condensation of protons/deuterons, condensed 4d/TSC unite together tightly to cause the cluster nuclear fusion according to the Takahashi's TSC nuclear fusion theory without collision against the atomic nucleus of the crystal lattice of the host metal or other one. 2 - 4 In the case of 4d/TSC by Li in the T site of Ni or Pd: 4d/TSC -» Be* -s- 2a + 47.6 MeV

(4)

Specially, the production of M* (A+8, Z + 4) by the reaction (2) and M* (A+12, Z + 6) by the reaction (3) can explain nuclear transmutations like 133 Cs into 1 4 1 Pr and 137 Ba into 149 Sm, respectively, which is indicated in the deuterium permeation experiments through alternating CaO and Pd layers by Iwamura et al.1 Moreover, consistent with his reports, replacing Ca with Mg in his experiments would occur with no nuclear absorption and nuclear transmutation of TSC/OSC because of being too light for Mg 2 + ion to recoil and collide 4d/TSC or 6d/OSC against the other nucleus, and no nuclear fusion because there would be too many valence (+2) and influential Mg 2 + ions to keep the symmetry of each polyhedron. This scenario about the formation of TSC/OSC can explain some of the experimental results of the electrolysis or deuterium permeation qualitatively, but it is based on many assumptions that must be proved experimentally or theoretically. And the hopping of the alkali or alkaline-earth metal ions and the recoil of H + / D + ions must be considered not only on the mass difference of each other but also on the other qualities. 3. Properties Derived from the Scenario Some properties are derived from the above scenario. Some of the major ones are as follows. 3.1. Three Kinds Flux

of Electrolytic

Current

Density

or

Deuterium

There are three kinds of electrolytic current density i or deuterium flux / , which have the minimum and maximum, respectively: (a) For permeation of H+/D+ ions: i h / d or f^. (b) For infiltration of alkali or alkaline-earth metal ions: iaik or /aik(c) For hopping of alkali or alkaline-earth metal ions: ihop or /hopGenerally, it may be that: 0 ~ (c) i ho p < (a) h/d < (b) iaik or 0 - (c) / h o p < (a) / h / d < (b) /aik-

(5)

540

However, these values might depend on the settings of experimental apparatus. Therefore, it might be necessary to control the value of the electrolytic current density or deuterium flux properly in experiments, for example in the high range for the preparation process of the permeation of H+/D+ ions and infiltration of the alkali or alkaline-earth metal ions first for a while, and then in the low range for the response process of the hopping of the alkali or alkaline-earth metal ions, condensation of protons/deuterons and nuclear reactions lastly. 3.2. Local Cooling Down due to Hopping Alkaline-earth Metal Ion

of Alkali

or

When the hopping of the alkali or alkaline-earth metal ion makes a cavity in the crystal lattice of the host metal, four H+/D+ ions at the vertexes of the tetrahedron or six H + / D + ions at those of the octahedron remain there constructing the surface of the cavity. In the analysis of the model of surface phonons, when one of the springs composing an infinite long one-dimensional diatomic lattice is cut off, the frequency of the lowest optical mode decreases to the Wallis mode. This explained using the Rayleigh's theorem described by the following equation: When the number m oscillator of infinite long one-dimensional lattice composed by f oscillators changes it's mass and spring constant, the motion of this one-dimensional lattice is described by the proper equation as follows.5

l/(au2-p)

/

+ J2^i/(MJu;2-CJ)=0

(6)

.7 = 1

a: change of mass (3: change of spring constant to: frequency, My. mass of the number j oscillator, Cy. spring constant of the number j oscillator, 5rnj-. Kronecker's delta. By replacing z = u2 and Zj = w|, the equation F(z) = F\(z) — F2{z) = 0 transformed from Eq. (6) gives solutions which are indicated by intersections of Fi(z) = F2(z) on the graph, where / F1(z) = ^mj/(MjZ •? =

- Cj)F2(z) = - l / ( a z - /?).

(7)

!

If the mass and spring constant of number m oscillator change to become a = ~Mm < 0 and (3 = —Cm < 0 which means disappearance of them, respectively, the lowest frequency decreases and the highest one increases. Applying this relationship to the diatomic lattice system consisting of light H+/D+ ions and alkali or alkaline-earth metal ion and heavy host metal ions, it might be expected that the frequency of some mode of lighter H + / D + ions on the surface of the cavity decreased and the cavity was cooled down while the alkali or alkaline-earth metal ion hopped out by increasing of frequency. If the coherent

541

phonon of the crystal lattice of the host metal is caused by electromagnetic impulse simultaneously with or after the hopping-out of the alkali or alkaline-earth metal ion, and the coherent oscillation of phonon is just in the decreased mode, it might be possible to cool down the local region effectively, although the frequencies of only a few modes decrease almost 10 meV at the most.

4.

Conclusion

In this study we revealed the formation of T S C / O S C explained clearly by the processes by which alkali or alkaline-earth metal ions infiltrate into the host metal and hop onto the other sites of the crystal lattice of the host metal. T h e hoppingout of the alkali or alkaline-earth metal ion recoil the condensed protons/deuterons strongly, causing nuclear transmutation, or weakly, causing nuclear fusion. And we showed, the important roles of the alkali or alkaline-earth metal ions is to make the cavity in the crystal lattice of the host metal by hopping, which squeezes H + / D + ions and cools down the cavity to cause the condensation of protons/deuterons.

Acknowledgements T h e author wishes to t h a n k Professor Takahashi of Osaka University for valuable information and advice.

References 1. Y. Iwamura, T. Ithoh, M. Sakano, N. Yamazaki, S. Kuribayashi, Y. Terada, T. Ishikawa, and J. Kasadi, Low energy nuclear transmutation in condensed matter induced by D2 gas permeation through Pd complexes, Proc. ICCF11 (in press) http://www.lenrcanr.org/ 2. A. Takahashi, Deuteron cluster fusion and related nuclear reaction in metaldeuterium/hydrogen systems, Recent Res. Devel. Phys. 6, 1-28 (2005). 3. A. Takahashi: 3 He/ 4 He PRODUCTION RATIOS BY TETRAHEDRAL SYMMTERIC CONDENSATION, Proc. ICCF11 (in press) http://www.lenr-canr.org/ 4. A. Takahashi, Mechanism of deuteron cluster fusion by EQPET model, Proc. ICCFIO (in press) http://www.lenr-canr.org/ 5. T. Ohshima and Y. Ohtsuki (eds.), Surface Phonons, Front of Physics Vol. 30 (Kyoritsu, 1992) (in Japanese).

CALCULATIONS OF N U C L E A R R E A C T I O N S P R O B A B I L I T Y IN A CRYSTAL LATTICE OF L A N T H A N U M D E U T E R I D E

V . A . K I R K I N S K I I A N D Y U . A. N O V I K O V Institute of Mineralogy and Petrography, Siberian Branch of the Russian Academy of Sciences, Prospect Academy Koptyuga 3, Novosibirsk 630090, Russia E-mail: [email protected]

The dynamic model of electron orbitals deformation was previously devised for palladium deuteride. It has now been applied to calculate the probability of nuclear reactions of hydrogen isotopes in the crystal lattice of lanthanum deuteride. In a series of computer simulations, the probability of D—D approach for random initial conditions was calculated, when the initial energies of the approaching deuterons were set in the range of 0.001-9.0 eV. For each experimental value of D—D approach the reaction rate was calculated on the shifted Coulomb potential with the shift energy, which equals to the energy of screening. The mean distance of D - D approach on the whole series equals 0.19 A. More than 54% of all experimental values show an approach of deuterons at a distance smaller than 0.1 A. The average reaction rate for the given set of the initial conditions is 10 3 , 2 8 s _ 1 per DD pair. This is three orders of magnitude less than the analogous rate calculated earlier for palladium deuteride. Allowing for the higher D content and the higher number of adjacent tetrahedral sites in LaD3 as compared with PdDo, 6, an overall nuclear fusion rate in lanthanum deuteride will be only slightly lower than in palladium deuteride, that is, 1 0 ~ 1 2 - 1 0 - 1 4 s _ 1 per DD pair.

To achieve a more sophisticated understanding of the mechanism and peculiar features of nuclear reactions in condensed matter, it is very important to expand a circle of substances that have been investigated. However, direct experimental research of new materials involves considerable difficulties, as the observable effects only slightly exceed the sensitivity of instrumentation, or the background level. In this connection, a random search of all substances to find which ones can catalyze cold nuclear fusion would be labor consuming and ineffective, especially taking into account the variations of their physical state and impurity content. Although most research on nuclear reactions in metal have been done with palladium, the high price and limited quantities of this material hinder the practical use of it. From the foregoing, the importance of theoretical calculation for search of materials is clear - a search to find which materials can be activated to produce nuclear fusion at low energies. We conducted a simulation of nuclear reactions of deuterium in palladium crystal lattice based on a dynamic model of electron orbital deformation in which hydrogen atoms are located in octahedral sites of closely packed metal atoms. 1_4 The calculation results correspond within an order of magnitude to the experimental 542

543

measurements of excess energy output (see, e.g. Ref. 5 and reviews in Refs. 1 and 6). Later, using the same model, the rate of a nuclear reaction was calculated in a titanium deuteride, where deuterium atoms are situated in tetrahedral sites of a crystal lattice, and the limiting content corresponds to TiD2 crystal structure. 4 In the present paper, we calculate the probability of a nuclear interaction in lanthanum deuteride, in which deuterium atoms can reside both in octahedral and tetrahedral sites of closely packed lanthanum atoms forming the LaD3 crystal lattice. The high content of deuterium in lattice should be favorable for implementing a nuclear interaction. Studies of lanthanum deuteride are also valuable because based on them we can draw conclusions about analogous compounds of lanthanide elements and yttrium, which have a similar lattice with slightly diminished crystal lattice parameters. For calculations of probability of nuclear reactions of hydrogen isotopes in the crystal lattice of lanthanum deuteride the dynamic model of electron orbitals deformation (EODD) offered earlier for palladium deuteride was used. 1-3 The hydrogen isotopes predominantly occupy tetrahedral sites in the face-centered cubic lattice of lanthanum hydride. Symmetrical positions of deuterium atoms with respect to the edge connecting two adjacent tetrahedral sites in lanthanum were selected as initial conditions for numerical tests. The initial trajectory of lanthanum 6s-electron was set as an ellipse, in one of its focal points a nucleus of lanthanum atom with an effective charge Z\,& is located. The effective charge Z\,a is calculated from the potential of ionization and the maximum radial density of La 6s-orbital wave-function.7 The electron can be found also on ellipse-like trajectories, which are distinct from the most probable ones, at different electron distances from La atom nucleus at the apogee. The calculations were carried out also for such trajectories using different initial outer electron orbital radii (see below). In a series of computer simulations, the probability of D-D approach for random initial conditions was calculated in the initial energy range of 0.001-9.0eV of approaching deuterons (the potential barrier for diffusion of deuterium atoms in lanthanum is about 0.43 eV). The most favorable conditions of two deuterons approaching one another were determined by preliminary computer modeling1 within the framework of the described model to reduce the calculation time. For each experimental value of D-D approach the reaction rate was calculated on the shifted Coulomb potential with the shift energy, which is equal to the energy of screening. The series consists of 40,000 experimental values. The mean distance of D-D approach on the whole series equals 0.19 A, however, more than 54% of all experimental values show an approach of deuterons for a distance smaller than 0.1 A. If one considers the reaction rate at each case of approach, and then averages as a whole on the entire sample, the general reaction rate for the given set of the initial conditions will make 10 3 2 8 s _ 1 per DD pair. It is three orders of magnitude less than the analogous rate calculated earlier for palladium deuteride, 1_3 but more than 10 times higher than the rate calculated for titanium deuteride. 4

544

Results of these calculations show that probability of fusion reactions depends not only on initial distances between deuterons but also on the character of electron orbitals of metal atoms. In order to investigate the influence of the initial outer electron orbital radius on an efficiency of deuteron approaching, another set of simulations was carried out. In the second series the range of outer orbital radii (a - 0.4) ± 0.05 A was used instead of (a —0.2)±0.05 A in the fist series (were a is a half of distances between lanthanum atoms located at the vertex of tetrahedral sites). The results of the second series essentially differ from the first series ones. The mean distance of D-D approach on the series equals 0.25 A (Fig. 1).

0.0

1.0

2.0

3.0

4.0

5.0

6.0

7.0

8.0

9.0

Energy (eV)

Figure 1. Distribution of minimal distances of D—D approach during their counter motions on the boundary of the neighbor tetrahedral sites in lanthanum deuteride vs their initial kinetic energy.

More than 33% of all experimental values show an approach of deuterons at a distance smaller than 0.1 A. If one considers the reaction rate at each case of approach, and then one averages as a whole over the entire sample, the average reaction rate for the given set of the initial conditions will be 10 1,41 s _ 1 per DD pair. Comparing Figs. 2 and 3, one can see that at the energy < l e V the reaction rates in both cases are nearly equal, but at higher energy the dependence character differ. The D-D reaction rate in lanthanum deuteride has a reverse dependence on energy in comparison with palladium deuteride (see, Refs. 1-3). To optimize calculations the most favorable initial conditions were selected. To obtain the true results, calculated values should also be multiplied by a correction factor,1 which allows for the probability of the occurrence of these favorable conditions. When calculating this factor it is necessary to take into consideration the fact that the content of deuterium in lanthanum deuteride is six times higher than in palladium deuteride and the number of deuterium atoms in adjacent tetrahedral

545 4.5-1

3.5-

o CD

H ••R

2.54

24

1.5-

0.5-I 0

1

2

3

4

5

6

7

8

9

Energy range (eV)

Figure 2. Energy dependence of D-D reaction rate in lanthanum deuteride according to EODD simulations for the first series.

sites is 32 times higher than in adjacent octahedral sites in PdDo.s- Besides, in LaD3 there are closely spaced adjacent octahedral and tetrahedral sites occupied by deuterium. Thus, if it is possible to provide high mobility of deuterons in LaD3 crystal lattice, the reaction rate will be only slightly lower than the rate calculated earlier 1-3 and experimentally observed in palladium deuteride (see, e.g. Ref. 5 and reviews in Refs. 1 and 6).

4

5

Energy range (eV)

Figure 3. Energy dependence of D-D reaction rate in lanthanum deuteride according to EODD simulations for the second series.

546

Owing to the diminished parameters of crystal lattices of deuterides of other rare earth metals and yttrium, the reaction rate of a nuclear fusion in t h e m can be closely matched to the rate in palladium deuteride, i.e., 1 0 - 1 2 - 1 0 - 1 4 s _ 1 per DD pair. Since the cost of a n a t u r a l mixture of rare e a r t h metals is much lower t h a n the same weight of palladium, and rare earth metals are much more a b u n d a n t in n a t u r e t h a n palladium (and other platinum group metals), they are attractive perspective catalysts for nuclear fusion at low energies.

Acknowledgement This work was supported by the R F B R (Grant No. 05-05-64930).

References 1. V.A. Kirkinskii and Yu. A. Novikov, Theoretical modeling of cold fusion. Novosibirsk, Novosibirsk State University, 105 p. (2002). 2. V.A. Kirkinskii and Yu. A. Novikov, Numerical calculations of cold fusion rates in metal deuterides, in: Condensed Matter Nuclear Science (Xing Z. Li, ed. Proc. ICCF-9), 162 (2003). 3. V.A. Kirkinskii and Yu. A. Novikov, Modelling of dynamic screening effects in solid states, Europhys. Lett. 67, 362 (2004). 4. V.A. Kirkinskii and Yu. A. Novikov, Calculations of nuclear reactions probability in a crystal lattice of titanium deuteride, in Condensed Matter Nuclear Science (P. Hagelstein and S. Chubb eds. Proc. ICCF-10) (2005). 5. V.A. Kirkinskii, V.A. Drebushchak, and A.I. Khmelnikov, Excess heat release during deuterium sorption-desorption by finely powdered palladium deuteride, Europhys. Lett. 58, 462 (2002). 6. P. Hagelstein et al. New Physical Effects in Metal Deuterides (http://www.lenrcanr.org/acrobat/Hagelsteinnewphysica.pdf). 7. J.T. Waber and D.T. Cromer, J. Chem. Phys. 42, 4116-4123.

POSSIBLE C O U P L E D ELECTRON A N D ELECTRON N E U T R I N O IN N U C L E U S A N D ITS PHYSICAL CATALYSIS EFFECT ON D - D COLD F U S I O N INTO HELIUM IN Pd

MIKIO FUKUHARA MR Tohoku University, Sendai, E-mail: [email protected].

Japan ac.jp

We investigate a possibility of coexistence of an electron and an electron neutrino in nucleus, by normalization of electroweak interaction. Provided that the electron of atom takes one's share of both electromagnetic and weak interactions, we obtain 2.07 x 10 — 5 eV as the electron mass for the weak one, from Compton wavelength. This value is close to estimated neutrino mass, 10~ 5 — 10 —6 eV, giving a possible answer for an unexplained problem of the standard model in particle physics. Thus, we can see that one electron and one neutrino exist in proton and neutron, respectively. Physical roles of electron and neutrino for cold fusion of helium in solid lattice were investigated in terms of elemental particle physics. The electron and neutrino in nucleus enhances the fusion reaction, based on weak interaction in 13 decays, as well as a catalytic effect of neutral pions.

1. Introduction An atomic nucleus is composed of neutrons and protons, but we cannot find electrons and neutrinos in the nucleus at the first glance. However, it has been recognized that these light particles, which are lepton with isospin 1/2, do not contain originally in nucleus, but generates certainly in nuclear transmutation processes such as /3 decay and helium formation in sun. Since a composite model, which the nucleus is composed of proton and electrons, was knocked out by discovery of neutron, wide credence has been given to a fixed concept that the electrons cannot exist in nucleus. 1 However, as far as the nucleus is constituent element of the atom, the distribution of the electron in nucleus is not perfectly zero without violation of uncertainty principle in spite of its extremely small volume. On the other hand, generation process for neutrino has not been entirely resolved. We have another look at the generation process. Our first interest lies in studying a possibility of coexistence of electrons and neutrinos in nucleus from a new angle on particle physics with lower energy. Although the neutrinos have three families or three flavor eigenstates (ye,v^ and vT) associated with the three charged leptons: the electron, the muon and the tau, we use the electron neutrino with the lightest mass in this study. As far as we know, no previous research has been done on coexistence of electrons and neutrinos in nucleus, except for nuclear reaction of excited electron and neutrino in solids.2 547

548

Next, we investigate an enhancement effect by the coupled electron and neutrino for nuclear cold fusion, in addition to catalytic effect of neutral pions. showed that the formation of helium nucleus from In the previous paper; two deuterons, i.e., fusion, requires necessarily a direct force due to exchange of two neutral pions which do not actually compose the deuteron nucleus. D 2 + D 2 + 2^° = He 4 .

(1)

The neutral pion is provided by two photons, which are produced by emission of excited collective electrons derived from the palladium atoms. The introduction of the pions makes possible to reduce remarkably an internuclear distance, enhancing fusion rate for helium formation. For a significant role for nuclear fusion by neutral pion, we explained that the pion could easily enter within effective nuclear force field of deuteron pairs at close proximity, because the neutral pion does not experience a Coulomb barrier. 4 Then we investigated necessary and sufficient conditions for cold fusion of helium in solid lattice in terms of elementary particle physics, using the Heisenberg uncertainty relation is given by the Yukawa formula: L < cAtzi

h/mpc,

(2)

5

where c is the velocity of light and t is time. The interaction for deuterium atom pairs is schematically shown in Fig. 1, along with charge pion-mediated pn interaction in deuteron. P

(3)

Figure 1. Schematic representation of electromagnetic interaction, p + e p + e , mediated by photon 7 for two deuterium atoms, D2, where p and n are proton and neutron, respectively.

The Pd lattice for confinement of deuteron pairs plays the same role as magnetic field confinement in hot nuclear fusion, because the attractive interaction between deuterium atom and electron is mediated by massive photon with 5.2 keV.

549

On the other hand, nitrogen in the earth's atmosphere was interpreted by endothermic nuclear transmutation of carbon and oxygen nuclei confined in carbonate lattice of the mantle, with help of electropionic attraction effect due to the excited electron and plenty of neutrinos. 6 However, it is not necessarily clear physical role of the electron and electron neutrino for nuclear fusion yet. 2. Coupled Electron and Neutrino in Electroweak Interaction For the generation of neutrinos and electrons, the /3-decay is the most familiar physical phenomenon. The following relation of the /3-decay describes a weak interaction between lepton and nucleon;7 n + v p + e~.

(4)

This formula shows that four particles form two groups; (n, v) with neutral charge and (p,e~) with charge. Since p and n have the quark structure uud and ddu, respectively, we can rewrite Eq. (4) as the form: d + v p + e~.

(5)

Equation (5) indicates that four elementary particles form two groups; (d, v) and (u, e~). In this formula, barion and lepton numbers, and charge (—1) are preserved before and after reaction. As far as quarks are permanently confined inside the nucleons, we must consider the interaction in narrow region of the nucleus. However, as a matter of fact, Eq. (5) has been treated in utter disregard of the above-mentioned physical condition. Then we consider conformation of Eq. (5), in terms of standard model in particle physics. Fermi elementary particle interaction between proton and neutron is shown in Fig. 2, using Feynman diagram. For this purpose, we use the lightest deuterium nucleus with one proton and one neutron, as a representative one. In Fig. 2, the weak interaction of Eq. (5), which involves exchange of electric charge, is mediated by charge intermediated vector boson, W between u and d quarks in different nucleon each other. On the other hand, both neutrino and antineutrino v in proton and both electron and antielectron e + in neutron are mediated by neutral intermediate boson, Z°: v + v e~ + e + . ±

(6) 8

Here, since masses of W and Z bosons are extremely large, 80.375 and 91.187 GeV,9 respectively, we can calculate their Compton wavelengths; 2.46 and 2.16 x 10~ 18 m, respectively. Thus, two group particles (u,e~) and (d, v) must bind together by weak force in very narrow region of around (2.2 — 2.5) x 10~ 18 m. For proton, the total positive charge (+1) of three quarks cancels the negative charge (+1) of the electron, while the neutron has positive and negative electrons for a total electric charge of zero. As a result, we can see that one electron and one neutrino exist in proton and neutron, respectively. Furthermore, v and e~ are coupled as an s-wave boson of spin 0, because the electroweak force requires that the spins are

550

Neutron

Proton

Figure 2. Schematic representation of elementary particle interactions, d + v u + e~ and e~ +v ^ e+P, mediated by W and Z° bosons in proton and neutron deuterium atom, respectively, where u and d are up and down quarks, respectively. The reaction, e _ -\-v e~ +v, is eliminated.

opposed to each other due to boson exchange. 10 Since the size of both lepton and quark is less than 1 0 _ 1 8 m and the nucleus size is around 10~ 15 m, we can assume that u and d quarks are surrounded by spherically symmetrical ball of electron and neutrino blurred by a time-exposure of its rapid motion in nucleus, respectively. Furthermore, although the standard model in particle physics does not specify how many quark-lepton pairs constitute the family,11 a limit number exists, as far as we treat natural atomic elements with atomic number up to around 110; three pairs must assign for one proton-neutron pair. In other words, the three kinds of pairs must intrinsically assign for one proton-neutron pair, but this problem has been overlooked in the high-energy particle physics. 3. Electron Distribution in Electroweak Interaction In the previous section, with a view to explaining coexistence of electron and neutrino in nucleus, a necessary role of weak interaction was shown. Notwithstanding the necessary condition, we feel a new question why the existence of electrons in proton does not violate uncertainty principle. Next, we consider a possibility of existence of electron in proton in terms of electroweak interaction. If light particle such as electron exists in nucleus, it cannot be generally confined in the nucleus because of large uncertainty of the momentum. However, the uncertainty determining the position of the electron in nucleus decreases as speed of the electron increases. This means probability of existence for electron in nucleus is not zero. In atom, nucleus and electrons are bound together by electromagnetic force of mediated photon (Fig. 1) for two deuterium atoms, D 2 . In general, the strength of force for boson exchange interaction is in proportional to square of an effective interacting zone of boson or in inverse proportion to square

551

of boson mass. In calculation of the strength for photon, we cannot make use of the latter's relation, because of photon with zero mass. Since Compton wavelength of the electron is 3.86 x 1 0 - 1 3 m, we can use the wavelength as the interacting zone of photon. Similarly, Compton wavelength, i.e., the interacting zone, of the W boson in weak interaction is 2.46 x 10~ 18 m. Thus the zone ratio of the electromagnetic interaction to the weak one is around 4.04 x 1 0 - 1 1 . Here, since one electron corresponds to one proton in atom, we can assume that the electron of atom takes one's share of both electromagnetic and weak interactions in proportional to the effective zone ratio in normalization of electromagnetic and weak interactions in regardless of their coupling constants. In other words, the weak force mediator is lodged with the (u, e~) group for a brief time. From the effective zone ratio, we can obtain 2.07 x 1 0 - 5 eV as the electron mass associated with the weak interaction. This value is close to the electron neutrino mass, 10~ 5 —10 -6 eV, 12 extrapolated from masses of muon and tau neutrinos obtained in Super-Kamiokande collaboration. This indicates that the ratio of the lepton mass is almost equivalent to the ratio of quark ones, giving to a possible answer for an unexplained problem of the standard model in particle physics, which the ratio of lepton mass within the first family is so large compared with the ratio of quark ones. And we can also reply why only the first family is needed to make up the ordinary protons, neutrons and electrons in the universe? The electrons and neutrinos coexist with quarks in "nucleon vessel" of atom which is firmly bound by electromagnetic interaction. On the other hand, the other two families exist only ephemerally after the electrons are completely separated from the nucleus by high-energy collisions. Although nuclear behaviors at low temperature have not aroused researcher's interest, because most nuclei have enormous energy of the order of a few MeV, we cannot ignore the role of the electrons for atoms associated with u and d quarks in particle physics. Further study for this interesting area is called for. 4. Physical Role of Electrons and Electron Neutrino for Nuclear Fusion In the previous section, we reported a possible coexistence of an electron and an electron neutrino in nucleus, based on weak interaction in /3-decay. Provided that the electron of atom takes one's share of both electromagnetic and weak ones according as the zone ratio, we can see that one electron and one neutrino exist in proton and neutron, respectively. When a helium atom is formed two deuterons, quarks, electrons and neutrinos must be mediated by charged and neutral intermediated bosons, W and Z° (Fig. 3), respectively, as a result of mediation of charged and neutral pions. u + e~ d + v,

(7)

+

e + v ^> e~ + u,

(8)

e~ + v

•.s I

(a)

^ ,

K1

•

•'-''/' - 1 _•

• (I

: »

•

"-'#"2»'-

(d)

(e)

# : Proton o : Neutron

Liquid-crystal nucleus structure of 55 3 Cs.

ilCsfT, C, O, ID] - [T] - [T, C, O, I - 7] - [O] - [T, C, O, I, D] = (25n + 25p)(2n + 2p)(23n)(3n + 3p)(25n + 25p).

(10)

The third term from the left hand side of Eq. (8) represents the outermost shell, which in terms of Platonic structures is an icosahedron, indicated here as an I-polyhedron. As shown here, its configuration has been stripped of seven crystalline nucleons (here neutrons). The state in which the two 2D units in Eq. (8) react is indicated by Eq. (9). ^ 2 ( n + p) + 2(n + p) + 1 ^ C s , = (25n + 25p)(2n + 2n + 2p + 2p)(23n)(2n + 2p + 3n + 3p)(25n + 25p).

(11) (12)

Equation (10) depicts the state in which the 2D units in the second (b) and fourth (d) blocks of the nucleons of the 1 | | C s nucleus have undergone liquid-crystal fusion. Because items (b) and (d) have fewer protons than the other items, proton reaction is small. Item (c) is a crystal composed solely of neutrons and lacking protons, and so because it has no power to attract the neutrons of the liquid-crystal compound nucleus 2(n+p), the 2(n+p) block is the result of reaction between (b) and (d). Its shell structure cannot be explained in terms of Victor Weisskopf's

568

Platonic structures. Further, under the solar-system model of the atomic nucleus, the reaction between (b) and (d) seen here cannot be produced by proton reaction. = (25n + 25p)(4n + 4p)(23n)(2n + 2p + 3n + 3p)(25n + 25p),

(13)

141 P r [ T , C , 0 , I , D ] - [ C M T , C , 0 , I - 7 ] - [ T , O M T , C , 0 , I , D ] . 59

(14)

Equation (11) indicates the change in the numbers of protons and neutrons that occur due to nuclear reaction in the blocks within the atomic nucleus. In the atomic nucleus that has undergone nuclear change to become ^gPr, indicated by Eq. (12), in the second block, (2n+2p) has become (4n+4p), indicating that the T-polyhedron (tetrahedron) has reacted to the C-polyhedron (cube) and changed. Similarly, in the fourth block, (2n+2n) has become (2n+2p+3n+3p), indicating that the O-polyhedron (octahedron) has changed to a T-polyhedral structure in the inner shell and an O-polyhedral structure in the outer shell. This is as shown in Fig. 3.

4 m, • m * * * • • *

: :

i ! .

*++

"

•••

• •

. ! ! . ! :

« *%•

7 . " ' - . ,T

'- • •

'

• • . . . ; •

•

•

•

•"#'-•

. ' . . - . - .

•::

;:


;. ' . . ' / / ' . . .

•

: :

,,«*

v

• ** ' . .

* P

C r, therefore making use of the r value as the size of the "atom" will result in the lower-bound estimate of A. By way of illustration, Table 2 present the number of events with the size r and the number of collisions I from the different ranges; AN* is the total number of events with I from these ranges. Table 1. Sizes of D* "atoms" at the apogee of r and at the perigee r m j n in units of 1 0 - 1 1 cm. I is the number of electron collisions with D* I r ^min

88 0.87 0.22

83 1.17 0.41

84 1.27 0.19

82 1.38 0.88

25 1.64 0.12

89 1.69 0.11

79 1.78 0.08

56 1.81 0.19

98 1.82 0.88

51 1.99 0.38

Figure 1 shows the functions X(l,l) and A(a). Averaging A (a) over a < Zmax, equivalent to the time averaging yields A f» 2 x 1 0 _ 4 s ^ 1 , which is 106 times greater than the value obtained in Refs. 1 and 2 on the basis of the dynamic model of electron orbital deformation (EODD). Taking into account that A(a) somewhat increases with the increase in a, the obtained average A should be treated as a lower-bound estimate. The contribution of 370 events presented in Table 2 to the

586 Table 2. Ranges of I

1-20 21-40 41-60 61-80 81-100

AN*

177731 114983 66531 39042 22461

Number of events with r and I from the indicated ranges Ranges of size r of the D* "atom" in units of 1 0 ~ n cm 0.5-1

1-1.5

1.5-2

2-2.5

2.5-3

3-3.5

3.5-4

4-4.5

4.5-5

0 0 0 0 1

0 0 0 0 3

0 1 2 1 2

0 5 10 3 2

2 4 9 7 2

4 14 16 13 3

7 19 23 17 8

2 25 25 10 11

0 43 36 22 18

obtained value of A is 99%, including the contribution of 10 events from Table 1 amounting to about 80 %. The application of classical mechanics usually provokes objections because classical mechanics enables one to put a shielding charge at any point and impart it any initial velocity (e.g., zero velocity). We deem it therefore important to emphasize that the equiprobable initial conditions we employed correspond to the real-life situation. In addition, the applied approach, which could be called the Bohr approach, is not a purely classical one, since the radiation has been "turned off". Quantummechanical models allowing for elastic processes only give a sufficiently accurate description of real physical processes for a very wide range of phenomena. It should be noted that from the quantum-mechanical viewpoint, D* is not a kind of a hypothetical atomic state with energies lower than that of the ground state. D* should be treated as an unsteady structure within many-particle nonradiating system.

1E+0 i

1E-1 1E-2 r

1E-5

1E-7

_

1E-8 1E-9 1E-10

^P ¥ J ! «

xr'

1E-6

-

I

-/

,A

1E-3 1E-4

/'

'•

1 \'=:

HP

'

r /

h

0

i

20

40

60

i

i

80

100

/, a

Figure 1.

Reaction rate. Dashed line denotes X(l,l)\ solid line designates A(a).

587

References 1. V. A. Kirkinskii and Yu.A. Novikov. Theoretical Modelling of Cold Fusion (Novosibirsk State University, Novosibirsk, 2002), p. 105. 2. V. A. Kirkinskii and Yu.A. Novikov, Europhys Lett 67, 362 (2004). 3. R. H. Fowler and E. A. Guggenheim Statistical Thermodynamics (Cambridge University Press, Cambridge, 1939).

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Author Index

A

F Falcioni, F., 377 Fauvarque, J.-F., 80 Fiore, R., 145 Fisher, J. C , 516 Fontana, F., 377 Frisone, F., 494 Fujii, M., 133 Fukuhara, M., 547 Furuyama, Y., 272

Adamenko, S. V., 356 Almaviva, S., 351 Amini, F., 163 Andreassi, V., 377 Aoki, Y., 253 Apicella, M., 117, 264 Arata, Y., 44

B

G

Ban, M., 411, 555 Bertolotti, M., 55

Gamberale, L., 377 Garbelli, D., 377 Gareev, F. A., 504 Gavritenkov, D. V., 231 Giacinti, O., 377 Goncharov, A. I., 582

c Cai, N. N., 482 Cao, D. X., 482 Capobianco, L., 117, 145 Castagna, E., 55, 117, 145, 156, 264, 351 Castano, C. H., 367 Celani, F., 289, 377, 404 Celia, E., 377 Chaudhary, I., 527 Chubb, S. R., 430 Chubb, T. A., 473 Clauzon, P. P., 80

H Hagelstein, P. L., Haque, M., 314 Higashizawa, M., Hubler, G., 264

441, 527 196

I Iizumi, K., 133 Ishikawa, T., 178 Itagaki, M., 188, 196 Itoh, T., 178 Iwai, H., 272 Iwamura, K., 178, 289

D D'Agostaro, G., 377 D'Aulerio, L., 117, 145 Dardik, I., 55 Dash, J., 86, 140 Del Prete, P. R., 145 Desyatov, A. V., 97 Di Stefano, V., 377, 404

K Kamiya, N., 133 Karabut, A. B., 214, 344

589

590

Kim, Y. E., 462 Kirkinskii, V. A., 542, 582 Kitamura, A., 272 Koldamasov, A. I., 97 Kornilova, A. A., 97, 206 Kornilova, J., 206 Kowalski, L., 171 Kuribayashi, S., 178 Kurihara, S., 196

L Lalleve, G. J.-M., 80 Lesin, S., 55 Li, X. Z., 26, 75, 278, 482 Lipson, A., 314 Lipson, A. G., 293, 304, 325, 336, 367 Little, S., 171 Liu, B., 75, 278, 482 Luce, G., 171 Lyakhov, B. F., 293, 304, 367

M Mancini, A., 377 Marchesini, M., 377 Marini, P., 377, 404 Marolo, T., 351 Mastromatteo, U., 377 Mazzitelli, G., 117 McConnell, D. B., 97 McKubre, M., 55, 117, 145, 264 McKubre, M. C. H., 392 Miley, G. H., 34, 293, 314, 325, 336, 367 Mitin, A. V., 367 Mitsushima, S., 133 Miura, H., 536 Mizuno, T., 65, 253 Momota, H., 325 Montereali, R. M., 351 Moretti, S., 55

Mueller, N., 75, 278 Muromtsev, V., 571

N Nakamura, M., 377 Narita, S., 188, 196, 284 Nishio, R., 272 Novaro, E., 377 Novikov, Y. A., 542 Numata, H., 411

o Odashima, T., 196, 284 Oehre, H., 75, 278 Ohmori, T., 253, 284 Ota, K.-L, 133

P Paoloni, S., 156 Percel, I., 314 Platonov, V., 571 Purchi, E., 377

Q Quercia, P.,

377

R Righi, E., 377 Rodionov, B., 421 Romer, M., 314 Rosada, A., 117, 264 Roussetski, A. S., 293, 304, 336

s Sakano, M., 178 Santoro, E., 117, 264 Sarto, F., 55, 117, 156, 264, 351 Satoh, R., 272 Saunin, E. I., 293, 304, 336

591

Savvatimova, L, 421, 571 Savvatimova, I. B., 231 Sawada, H., 196 Schoch, P., 75, 278 Shimadu, S., 284 Shrestha, P. J., 34 Sibilia, C , 55, 117, 156, 264, 351 Slaughter, R., 171 Sona, P. G., 377 Spallone, A., 377, 404 Storms, E., 108

T Takahashi, A., 1, 289, 454 Takahashi, D., 188 Taniguchi, S., 188, 196, 284 Taniike, A., 272 Tanzella, F., 55, 117, 145, 264 Tanzella, F. L., 392 Tashirev, A. B., 206 Terada, Y., 178 Teshima, N., 284 Todarello, F., 377 Toriyabe, Y., 65, 253 Trenta, G., 377 Tsivadze, A. Y., 367 Tsuchiya, K.-L, 521

U Ushirozawa, T.,

196

V Vincenti, M. A., 351 Violante, V., 55, 117, 145, 156, 264, 351 Vysotskii, V. I., 97, 206, 356

w Wagatsuma, Y., 188 Wang, Q., 86, 140 Wei, Q. M., 75, 278, 482

Y Yabuuchi, N., 564 Yamada, H., 188, 196, 284 Yamamoto, H., 577 Yamazaki, N., 178 Yang, H. I., 97 Yang, Y., 314

z Zhang, W.-S., 86 Zhang, Y.-C., 44 Zheng, S. X., 482 Zhidkova, I. E., 504 Zilov, T., 55 Zubarev, A. L., 462

Recent progress in the emerging field of condensed matter nuclear science (CMNS) is presented as a combination of basic nuclear science, energy, nanomaterials science, electrochemistry and nuclear physics. Key and selected papers from an important conference in this exciting area provide the latest advances in CMNS studies. Current results from cold fusion and condensed matter nuclear science are included.

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