Search for Nuclear Reaction Products in Gas Phase Experiments - Deuterium Permeation and Absorption -

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Session 3 O_2 Nuclear Measurements (I) Search for Nuclear Reaction Products in Gas Phase Experiments - Deuterium Permeation and Absorption - A. Kitamura 1, Y. Sasaki 1, Y. Miyoshi 1, Y. Yamaguchi 1, A. Taniike 1, Y. Furuyama 1, A. Takahashi 2, R. Seto 2, and Y. Fujita 2 1 Division of Marine Engineering, Graduate School of Maritime Sciences, Kobe University Higashinada-ku, Kobe 6580022, Japan 2 Technova Inc., Chiyoda-ku, Tokyo 1000011, Japan Employing both in situ and ex situ accelerator analyses, we have tried to replicate the nuclear transmutation [1] of Sr to Mo under deuterium permeation through a variety of multilayered CaO/Sr/Pd samples. Apparently positive results have been obtained in 8 runs out of 14, although the identification of Mo peaks in the PIXE analysis are not definite. It is implied that sputtering loss of the atoms could be responsible for the observed tendency that areal density of Sr decreases in most cases, while there is a modest increase in Mo. In addition to the accelerator analyses, -ray detection is tried for samples implanted with W atoms in expectation of transmutation from 183 W to radioactive 191 Pt. As another series of experiments, we intended to confirm heat and 4 He generation by deuterium (D) absorption in nano-sized Pd powders reported by Arata and Zhang [2], and to investigate the underlying physics. The experimental procedure and the results on the heat measurements will be discussed in detail in the following two presentations [3,4]. As will be explained there, nano-sized powder of mixed Pd and Zr oxides fabricated by Santoku Corp., Kobe, Japan, have revealed not only interesting mesoscopic effects but also large isotope effects both in the first phase (zero-pressure interval) and the second phase (with the pressure increasing up to the stationary value) of gas filling. In the latter half of the present paper, we discuss a possible cause of the large isotope effects mentioned above. For this purpose, detection of possible nuclear ash including charged particles as well as neutrons and gamma rays are tried. [1] Y. Iwamura, M. Sakano and T. Itoh: Jpn. J. Appl. Phys. 41 (2002) 4642-4650; Y. Iwamura et al.: Proc. ICCF12, 2005, Yokohama, Japan, (World Scientific Publishing Co. Pte. Ltd, 2006) 178-187. [2] Y. Arata and Y. Zhang: The special report on research project for creation of new energy, J. High Temperature Society, 2008, No. 1; Y. Arata, and Y. Zhang: Condensed Matter Nuclear Science, Proc. 12 th Int. Conf. on Cold Fusion (ed. A. Takahashi, Y. Iwamura, and K. Ota, World Scientific, 2006) pp.44-54. [3] Y. Sasaki, A. Kitamura, Y. Miyoshi, T. Nohmi, A. Taniike, A. Takahashi, R. Seto, and Y. Fujita: Anomalous Heat Generation in Charging of Pd Powders with High Density Hydrogen Isotopes, (I) Results of absorption experiments using Pd powders, this meeting. [4] A. Takahashi, A. Kitamura, Y. Sasaki, Y. Miyoshi, T. Nohmi, A. Taniike, R. Seto, and Y. Fujita: Anomalous Heat Generation in Charging of Pd Powders with High Density Hydrogen Isotopes, (II) Discussions on Experimental Results and Underlying Physics, this meeting. 30 ICCF-15

S3_O2 / ICCF15 Search for Nuclear Reaction Products in Gas Phase Experiments - Deuterium Permeation and Absorption - A. Kitamura 1, Y. Sasaki 1, Y. Miyoshi 1, Y. Yamaguchi 1, A. Taniike 1, Y. Furuyama 1, A. Takahashi 2, R. Seto 2, and Y. Fujita 2 1 Graduate School of Maritime Sciences, Kobe University, 2 Technova Inc.

[A] Elemental analysis of CaO/X/Pd multilayered samples subjected to deuterium permeation Iwamura et al. claimed [1] that nuclear transmutation occurs during forced permeation of deuterium (D) through a multi-layered film of X/CaO/Pd, with X being an element to be transmuted, e.g., 133 Cs transmuted to 141 Pr, 88 Sr to 96 Mo, etc. [1] Y. Iwamura, M. Sakano and T. Itoh; Jpn. J. Appl. Phys. 41 (2002) 4642. In addition to the modified version of the sample exposure system with reversed flow direction installed at a beam line of a tandem electrostatic accelerator 5SDH2, a stand-alone D permeation system was used to examine the phenomenon by in situ or ex situ PIXE/ERD analysis, respectively. [2] T. Yamaguchi, et al.; Paper 28, ICCF14, Washington D. C. Aug. 10-15, 2002. S3_O2 / ICCF15

S3_O2 / ICCF15 Sample holder Pd substrate Multilayered CaO/X/Pd Vacuum D permeation D 2 O-ring

S3_O2 / ICCF15 [A-1] Summary of PIXE analysis We tried to replicate the nuclear transmutation of Sr (2 50 10 15 cm -2 ) to Mo under deuterium permeation through a variety of multilayered CaO/Sr/Pd samples. Apparently positive results were obtained in 8 runs out of 14, although the identification of Mo peaks in the PIXE analysis was not definite. It has been implied that sputtering loss of the atoms could be responsible for the observed tendency that areal density of Sr decreases in most cases, while there is a modest increase in that of Mo.

S3_O2 / ICCF15 [A-2] Summary of radioactivity measurements Tungsten was also tested as the element X. Assuming the regularity in transmutation that (atomic number, mass number) increase by (4, 8), we expected production of radioactive nuclei 191 Pt (T 1/2 = 2.86 d) from 183 W. An NaI(Tl) scintillation probe and a HPGe detector were employed to detect 0.538-MeV gamma rays from 191 Pt. The result of the measurement for the first sample was not always positive; the areal density of 191 Pt is smaller than 10 7 cm -2, if any.

[B] Deuterium absorption by Pd nanoparticles S3_O2 / ICCF15 The second subject is to confirm heat and 4 He generation by D absorption in nano-sized Pd powders reported by Arata and Zhang [2], and to investigate the underlying physics. We have performed calorimetry during D 2 or H 2 absorption by micronized powders of Pd, Pd-black, and Pd-Zr oxide compounds (Santoku Corp.) using a twin system [3]. [3] Y. Arata and Y. Zhang; The special report on research project for creation of new energy, J. High Temperature Soc., No. 1, 2008. [4] A. Kitamura, T. Nohmi, Y. Sasaki, A. Taniike, A. Takahashi, R. Seto, and Y. Fujita; Anomalous Effects in Charging of Pd Powders with High Density Hydrogen Isotopes, Phys. Lett. A, 373 (09) 3109.

The experimental procedure and the results on the heat measurements have been and will be discussed in detail in the following two presentations [5,6]. [5] A. Takahashi, et al,: paper S2_O4, this meeting. [6] Y. Sasaki, et al.: paper S7_O5, this meeting. As explained there, nano-sized powder of mixed Pd and Zr oxides fabricated by Santoku Corp., Kobe, Japan, have revealed not only interesting mesoscopic effects but also large isotope effects both in the first phase (zero-pressure interval) and the second phase (with the pressure increasing up to the stationary value) of gas filling. In the latter half of the present paper, we discuss a possible cause of the large isotope effects mentioned above. For this purpose, detection of possible nuclear ash including charged particles as well as neutrons and gamma rays are tried. S3_O2 / ICCF15

A twin system for D/H absorption experiments S3_O2 / ICCF15 Vacuum gauge Pressure gauge D 2 gas cylinder H 2 gas cylinder A 1 system for D 2 run Vacuum pump A 2 system for H 2 run Reaction chamber

1.2 (c) Mixed oxides of Pd Zr 1.2 S3_O2 / ICCF15 Output power [W] 0.8 0.4 0 Power (D 2 ) Power (H 2 ) Pressure (D 2 ) Pressure (H 2 ) 0.8 0.4 0 Pressure [MPa] 0 500 1000 1500 Time [min] Fig. 3. Evolution of heat and pressure in the vessel after introduction of D 2 gas (blue/light blue) or H 2 gas (red/pink); (c) mixed oxides of Pd and Zr (D-PZ1#1 and H-PZ2#1).

S3_O2 / ICCF15 Conclusions for heat measurements -For Pd Zr oxide nano-powders, anomalously large energies of hydrogen isotope absorption, 2.4 0.2 ev/d-atom and 1.8 0.4 ev/h-atom, as well as large loading ratio of D/Pd =1.1 0.0 and H/Pd =1.1 0.3, respectively, were observed in the phase of deuteride/hydride formation (the first phase). -The sample charged with D 2 showed significantly positive output energy in the second phase after the deuteride formation.

S3_O2 / ICCF15 Functional view of the B system Super needle valve Si surface barrier detector (SSBD) or Ion implanted Si detector (IISD) Pressure gauge MCA Cold trap Vacuum gauge Retractable shield Pd ZrO 2 sample Thermo couple Heater D 2 Vacuum pump Vacuum pump Chiller

S3_O2 / ICCF15 6 discriminated 5 Pressure 0.15MPa Evacuation to 1.0MPa Counts 4 3 2 24-MeV alpha particles could be detected in this energy region with the SSBD acting as a E detector. 1 0 1 2 3 4 5 6 7 8 Energy [MeV] Spectra recorded by the SSBD with a 200- -thick depletion layer for D-PZ1#3B

Counting could be alphas of 5.75, 9.95, 12.8 MeV by minor branch of 4D fusion. But we cannot rule out the possibility of electrical noise by mechanical oscillation. 30 0.15 MPa 1 MPa 1.2 S3_O2 / ICCF15 Number of counts 20 10 0.8 0.4 Pressure (MPa) 0 5/29 5/30 5/31 6/1 6/2 6/3 6/4 Time Evacuation and re-pressurization Evolution of total counts in the 1-12 MeV range of the spectra measured by the SSBD (D-PZ1#3B) 0

1000 100 D-PZ14 D-PZ15 241Am S3_O2 / ICCF15 Yield 10 1 0 0 1 2 3 4 5 6 7 8 E (MeV) Spectra recorded by the IISD with a 500- -thick depletion layer in runs D-PZ14#1B and D-PZ15#1B-#2B.

1.0 baking D-PZ14#1B baking D-PZ15#1B&2B 100 S3_O2 / ICCF15 0.8 80 P (MPa) 0.6 0.4 0.2 60 40 20 T B (deg. C), Ch. particle count 0.0 21.00 22.00 23.00 24.00 25.00 26.00 Time (dd.hh) 0 Neutron Gamma PB (MPa) TB (deg. C) (4.7-5.6) MeV (1-8) MeV Evolution of pressure and IISD counting and other radiations during the runs D-PZ14#1B through D-PZ15#2B.

S3_O2 / ICCF15 -It has been turned out that the upper surface of the retractable shield has a 241 Am contamination, and the IISD could see the spot in case of insufficient retraction. -However, if the countings were of charged particles, we can estimate possible range of particle energy. p (MPa) 0.15 0.6 pl (mm atm) 22.5 90 p 4.74 4.85 E 2 = 4.7 MeV d t E 1 (MeV) 4.77 4.79 4.97 5.07 3 He 5.05 6.01 4 He 5.12 6.26 p 5.63 5.73 E 2 = 5.6 MeV d t E 1 (MeV) 5.66 5.68 5.83 5.92 3 He 5.91 6.80 4 He 5.98 7.02 Estimation of energy for assumed particles.

S3_O2 / ICCF15 [B] Summary of reaction product measurements in the system B for gas charging of PZ samples. We have observed several to several tens of counts in the 1 10 MeV range, which appeared to be emitted coincidentally with pressure change. However, we cannot rule out the possibility that they are due to electronic noise or contamination of 241 Am. Up to now, we have got no firm evidence of charged particle emission. We are planning detection of X-rays as one of the candidates for the reaction products.