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Journal Articles

Development of analytical techniques for isotopic composition determination of uranium particles in environmental sample for safeguards with Secondary Ion Mass Spectrometry

Tomita, Ryohei; Tomita, Jumpei; Suzuki, Daisuke; Yasuda, Kenichiro; Miyamoto, Yutaka

Hosha Kagaku, (48), p.1 - 15, 2023/09

Secondary Ion Mass Spectrometry (SIMS) is the method to detect secondary ions produced by the sputtering of primary ions. SIMS is one of effective method to measure isotopic composition of particles containing nuclear material in environmental sample for safeguards. We are a group member of the International Atomic Energy Agency (IAEA)'s network of analytical laboratories and have developed analytical techniques using SIMS and other mass spectrometers for nuclear safeguards. We will introduce the principle of SIMS and analytical techniques developed by our group to measure isotopic composition of uranium particles which having a particle diameter of micron order in environmental sample for safeguards.

Journal Articles

Analytical technique for isotope composition of nuclear micro particles

Miyamoto, Yutaka; Suzuki, Daisuke; Tomita, Ryohei; Tomita, Jumpei; Yasuda, Kenichiro

Isotope News, (786), p.22 - 25, 2023/04

no abstracts in English

Journal Articles

Multiple mechanisms in proton-induced nucleon removal at $$sim$$100 MeV/nucleon

Pohl, T.*; Sun, Y. L.*; Obertelli, A.*; Lee, J.*; G$'o$mez-Ramos, M.*; Ogata, Kazuyuki*; Yoshida, Kazuki; Cai, B. S.*; Yuan, C. X.*; Brown, B. A.*; et al.

Physical Review Letters, 130(17), p.172501_1 - 172501_8, 2023/04

 Times Cited Count:5 Percentile:92.42(Physics, Multidisciplinary)

We report on the first proton-induced single proton- and neutron-removal reactions from the neutron deficient $$^{14}$$O nucleus with large Fermi-surface asymmetry at $$sim$$100 MeV/nucleon. Our results provide the first quantitative contributions of multiple reaction mechanisms including the quasifree knockout, inelastic scattering, and nucleon transfer processes. It is shown that the inelastic scattering and nucleon transfer, usually neglected at such energy regime, contribute about 50% and 30% to the loosely bound proton and deeply bound neutron removal, respectively.

Journal Articles

Variation of crystallinity and secondary ion quantity of uranium particles with heating temperature of Sample preparation

Tomita, Ryohei; Tomita, Jumpei; Yomogida, Takumi; Suzuki, Daisuke; Yasuda, Kenichiro; Esaka, Fumitaka; Miyamoto, Yutaka

KEK Proceedings 2022-2, p.108 - 113, 2022/11

Automated Particle Measurement (APM) is the first measurement of environmental sample for safeguard purpose. APM tells us the number of particles in sample, their enrichment and their location. Precision and accuracy of APM is easily affected by particle condition. We have investigated how influential baking temperature in sample preparation are for uranium secondary ion quantity, uranium hydride generation and particle crystallinity. Our experimental results showed that baking temperature of 800$$^{circ}$$C reduced uranium secondary ion quantity to 33% compared with baking at 350$$^{circ}$$C. Uranium hydride generation ratio of the sample baked at 850$$^{circ}$$C was also 4 times higher than the sample baked at 350$$^{circ}$$C. Baking at 850$$^{circ}$$C raised only crystallinity of uranium particles. Baking sample at too high temperature caused less uranium secondary ion generation and much more uranium hydride generation. It made precision and accuracy of APM worse. In our experiment, baking at 350$$^{circ}$$C is suitable for uranium particles in the safeguards sample.

Journal Articles

Preparation of the particles containing isotope reference uranium for the determination of the low abundant U isotope ratios

Tomita, Jumpei; Tomita, Ryohei; Suzuki, Daisuke; Yasuda, Kenichiro; Miyamoto, Yutaka

KEK Proceedings 2022-2, p.154 - 158, 2022/11

Precise determination of minor U isotopes ($$^{233}$$U and $$^{236}$$U) of particles from the safeguard environmental samples is powerful method for detecting the undeclared nuclear activities. In this study, preparation method of U particle was examined to utilize for the minor U isotope determination. The porous silica particles were used as the particle matrix and lutetium was mixed to the impregnation solution as U impregnation indicator for the particle picking. The result of the Scanning Electron Microscope indicated that the contacting the solution with Si particles overnight gently could produce the impregnated particles effectively rather than the mixing them with PFA stick.

Journal Articles

Design and actual performance of J-PARC 3 GeV rapid cycling synchrotron for high-intensity operation

Yamamoto, Kazami; Kinsho, Michikazu; Hayashi, Naoki; Saha, P. K.; Tamura, Fumihiko; Yamamoto, Masanobu; Tani, Norio; Takayanagi, Tomohiro; Kamiya, Junichiro; Shobuda, Yoshihiro; et al.

Journal of Nuclear Science and Technology, 59(9), p.1174 - 1205, 2022/09

 Times Cited Count:6 Percentile:84.97(Nuclear Science & Technology)

In the Japan Proton Accelerator Research Complex, the purpose of the 3 GeV rapid cycling synchrotron (RCS) is to accelerate a 1 MW, high-intensity proton beam. To achieve beam operation at a repetition rate of 25 Hz at high intensities, the RCS was elaborately designed. After starting the RCS operation, we carefully verified the validity of its design and made certain improvements to establish a reliable operation at higher power as possible. Consequently, we demonstrated beam operation at a high power, namely, 1 MW. We then summarized the design, actual performance, and improvements of the RCS to achieve a 1 MW beam.

Journal Articles

Optimization of SIMS-APM for high enrichment uranium particles including higher uranium hydride

Tomita, Ryohei; Tomita, Jumpei; Yomogida, Takumi; Suzuki, Daisuke; Yasuda, Kenichiro; Esaka, Fumitaka; Miyamoto, Yutaka

KEK Proceedings 2021-2, p.146 - 150, 2021/12

no abstracts in English

Journal Articles

Age determination analysis of a single uranium particle for safeguards

Suzuki, Daisuke; Tomita, Ryohei; Tomita, Jumpei; Esaka, Fumitaka; Yasuda, Kenichiro; Miyamoto, Yutaka

Journal of Radioanalytical and Nuclear Chemistry, 328(1), p.103 - 111, 2021/04

 Times Cited Count:3 Percentile:45.99(Chemistry, Analytical)

An analytical technique was developed to determine the age of uranium particles for safeguards. After the chemical separation of uranium and thorium, the $$^{230}$$Th/$$^{234}$$U ratio was measured using single-collector inductively coupled plasma mass spectrometry and a $$^{233}$$U-based reference material comprising a certain amount of $$^{229}$$Th as a progeny nuclide of $$^{233}$$U. The results allowed us to determine the purification age of two certified materials, i.e., U-850 and U-100, which was in good agreement with the reference purification age (61 y). Moreover, the age of a single U-850 particle was determined with a difference of -28 to 2 years from the reference date.

Journal Articles

Crack expansion and fracturing mode of hydraulic refracturing from Acoustic Emission monitoring in a small-scale field experiment

Ishida, Tsuyoshi*; Fujito, Wataru*; Yamashita, Hiroto*; Naoi, Makoto*; Fujii, Hirokazu*; Suzuki, Kenichiro*; Matsui, Hiroya

Rock Mechanics and Rock Engineering, 52(2), p.543 - 553, 2019/02

AA2017-0694.pdf:2.54MB

 Times Cited Count:16 Percentile:67.51(Engineering, Geological)

We pressurized and injected water in a hole drilled downward from a floor of the 500 m level gallery in MIU, central Japan. Acoustic emissions (AEs) monitored with 16 sensors in four boreholes located 1 m away from the HF hole exhibited two-dimensional distributions, which likely delineate a crack induced by the fracturing. Expansions of the regions in which AEs occurred were observed only immediately after the first and second BDs. Many AE events in other periods were distributed within the regions where AE events had already occurred. The initial motion polarities of P-waves indicate that tensile-dominant AE events occurred when the regions expanded and they were distributed primarily on the frontiers of the regions where AE events had already occurred. The experimental results suggest that increasing the injection flow rate is effective for generating new cracks in the refracturing, with the new crack expansions being induced by tensile fracturing.

Journal Articles

Nuclear structure of $$^{76}$$Ni from the ($$p$$,$$2p$$) reaction

Elekes, Z.*; Kripk$'o$, $'A$*; Sohler, D.*; Sieja, K.*; Ogata, Kazuyuki*; Yoshida, Kazuki; Doornenbal, P.*; Obertelli, A.*; Authelet, G.*; Baba, Hidetada*; et al.

Physical Review C, 99(1), p.014312_1 - 014312_7, 2019/01

 Times Cited Count:10 Percentile:64.15(Physics, Nuclear)

The nuclear structure of the $$^{76}$$Ni nucleus was investigated by ($$p$$,$$2p$$) reaction using a NaI(Tl) array to detect the deexciting prompt $$gamma$$ rays. A new transition with an energy of 2227 keV was identified by $$gamma gamma$$ and $$gamma gamma gamma$$ coincidences. Our shell-model calculations using the Lenzi, Nowacki, Poves, and Sieja interaction produced good candidates for the experimental proton hole states in the observed energy region, and the theoretical cross sections showed good agreement with the experimental values. Although we could not assign all the experimental states to the theoretical ones unambiguously, the results are consistent with a reasonably large Z = 28 shell gap for nickel isotopes in accordance with previous studies.

Journal Articles

Accurate sensitive analytical technique of ultra-trace plutonium in the IAEA environmental samples

Miyamoto, Yutaka; Yasuda, Kenichiro; Suzuki, Daisuke; Esaka, Fumitaka; Magara, Masaaki

KEK Proceedings 2017-6, p.292 - 298, 2017/11

Our updated analytical techniques of ultra-trace plutonium in the IAEA environmental samples by ICP-MS were mentioned. Some careful techniques to accurately determine ultra-trace plutonium in the range of femto-grams to pico-grams were introduced. The uncertainties of analytical results were estimated according to the GUM concept. Our trials of determination of sub-femto grams americium in an environmental sample were also mentioned.

Journal Articles

Analysis of plutonium isotope ratios including $$^{238}$$Pu/$$^{239}$$Pu in individual U-Pu mixed oxide particles by means of a combination of alpha spectrometry and ICP-MS

Esaka, Fumitaka; Yasuda, Kenichiro; Suzuki, Daisuke; Miyamoto, Yutaka; Magara, Masaaki

Talanta, 165, p.122 - 127, 2017/04

 Times Cited Count:15 Percentile:52.34(Chemistry, Analytical)

The isotope ratios of $$^{238}$$Pu/$$^{239}$$Pu, $$^{240}$$Pu/$$^{239}$$Pu, $$^{241}$$Pu/$$^{239}$$Pu, and $$^{242}$$Pu/$$^{239}$$Pu were measured for individual Pu and U-Pu mixed oxide particles by a combination of alpha spectrometry and inductively coupled plasma mass spectrometry (ICP-MS). As a consequence, we were able to determine the $$^{240}$$Pu/$$^{239}$$Pu, $$^{241}$$Pu/$$^{239}$$Pu, and $$^{242}$$Pu/$$^{239}$$Pu isotope ratios with ICP-MS after particle dissolution and chemical separation of uranium, plutonium and americium with UTEVA resins. Furthermore, $$^{238}$$Pu/$$^{239}$$Pu isotope ratios were able to be calculated by using both the $$^{238}$$Pu/($$^{239}$$Pu+$$^{240}$$Pu) activity ratios that had been measured through alpha spectrometry and the $$^{240}$$Pu/$$^{239}$$Pu isotope ratios determined through ICP-MS. Therefore, the combined use of alpha spectrometry and ICP-MS is useful in determining plutonium isotope ratios, including $$^{238}$$Pu/$$^{239}$$Pu, in individual U-Pu mixed oxide particles.

Journal Articles

Evidence for a new nuclear "magic number" from the level structure of $$^{54}$$Ca

Steppenbeck, D.*; Takeuchi, Satoshi*; Aoi, Nori*; Doornenbal, P.*; Matsushita, Masafumi*; Wang, H.*; Baba, Hidetada*; Fukuda, Naoki*; Go, Shintaro*; Homma, Michio*; et al.

Nature, 502(7470), p.207 - 210, 2013/10

 Times Cited Count:285 Percentile:99.78(Multidisciplinary Sciences)

no abstracts in English

Journal Articles

QA/QC activities and estimation of uncertainty for ultra-trace analysis of uranium and plutonium in safeguards environmental samples

Usuda, Shigekazu*; Magara, Masaaki; Esaka, Fumitaka; Yasuda, Kenichiro; Kokubu, Yoko; Lee, C. G.; Miyamoto, Yutaka; Suzuki, Daisuke; Inagawa, Jun; Sakurai, Satoshi; et al.

Journal of Nuclear and Radiochemical Sciences, 11(2), p.A5 - A9, 2011/01

In the analysis of IAEA safeguards environmental samples, isotope ratios of ultra-trace amounts of uranium and plutonium in samples taken from nuclear facilities are determined to detect undeclared nuclear materials and activities. In order to keep and enhance the reliability of the measurement results, validation of analytical methods and estimation of measurement uncertainty in such ultra-trace analysis should be properly done in accordance with worldwide standards. In this paper, the current activities on achievement of QA/QC (quality assurance and quality control) and estimation of measurement uncertainty in the ultra-trace analysis at a clean chemistry laboratory (CLEAR) of JAEA are reported.

Journal Articles

The Project for grouting development for high level radioactive waste repository, 2; Relationship between basic properties and penetrability of low-alkaline cementitious grout material

Suzuki, Kenichiro*; Miura, Norihiko*; Iriya, Keishiro*; Noda, Masaru*; Kishi, Hirokazu

Doboku Gakkai Heisei-22-Nendo Zenkoku Taikai Dai-65-Kai Nenji Gakujutsu Koenkai Koen Gaiyoshu (DVD-ROM), p.85 - 86, 2010/09

no abstracts in English

Journal Articles

Research and development on environmental radionuclides for nuclear non-proliferation at Japan Atomic Energy Agency

Usuda, Shigekazu; Shinohara, Nobuo; Sakurai, Satoshi; Magara, Masaaki; Miyamoto, Yutaka; Esaka, Fumitaka; Yasuda, Kenichiro; Kokubu, Yoko; Hirayama, Fumio; Lee, C. G.; et al.

KEK Proceedings 2007-16, p.13 - 22, 2008/02

For the purpose of controlling and monitoring radiations and radioactive materials emitted from nuclear facilities to the environment and also evaluating their effects, various R&D on environmental radioactivity has been carried out at Japan Atomic Energy Agency (JAEA). Especially, for the abolition of nuclear weapons and for peaceful uses nuclear energy, ultra-trace analysis of environmental samples for safeguards and ultra-high sensitive monitoring of radionuclides for the CTBT verification, which have been scheduled in the middle of 1990s, have been promotted under the auspices of the Japanese Government at JAERI, the former of JAEA. In this presentation, the outline of R&D on environmental radioactivity for nuclear non-proliferation is introduced. In addition, applications of the developed techniques and future perspectives will be discussed.

Journal Articles

Development of analytical technique for safeguards environmental samples at JAEA; Current status and development of analytical method for isotope ratios of plutonium particles

Magara, Masaaki; Usuda, Shigekazu; Sakurai, Satoshi; Shinohara, Nobuo; Esaka, Fumitaka; Kokubu, Yoko; Suzuki, Daisuke; Yasuda, Kenichiro; Lee, C. G.; Inagawa, Jun; et al.

Kaku Busshitsu Kanri Gakkai (INMM) Nihon Shibu Dai-29-Kai Nenji Taikai Rombunshu (CD-ROM), 6 Pages, 2008/00

JAEA has been developing, under the auspices of the Ministry of Education, Culture, Sports, Science and Technology of Japan, analytical techniques for ultra-trace amounts of nuclear materials in the environmental samples in order to contribute to the strengthened safeguards system. In January 2003, JAEA was qualified as a member of the IAEA network analytical laboratories (NWAL) for environmental sample analysis. Since then, JAEA has conducted the analysis of domestic and the IAEA samples. Two techniques, bulk and particle analyses, are available for the environmental samples and the latter method generally provides more detailed information about history of nuclear materials in a facility. However, isotope ratios of uranium are measured in the particle analysis at present and it is wished to develop analytical method for isotope ratios of plutonium in individual particles. We commence the development of the plutonium particle analysis and the consideration of age-dating for plutonium particles through the atomic ratio of Pu-241 and Am-241.

Journal Articles

Development of safeguards environmental sample analysis techniques at JAEA as a network laboratory of IAEA

Sakurai, Satoshi; Magara, Masaaki; Esaka, Fumitaka; Hirayama, Fumio; Lee, C. G.; Yasuda, Kenichiro; Inagawa, Jun; Suzuki, Daisuke; Iguchi, Kazunari; Kokubu, Yoko; et al.

STI/PUB/1298 (CD-ROM), p.791 - 799, 2007/08

no abstracts in English

Journal Articles

Development of analytical techniques for safeguards environmental samples at JAEA

Sakurai, Satoshi; Magara, Masaaki; Usuda, Shigekazu; Watanabe, Kazuo; Esaka, Fumitaka; Hirayama, Fumio; Lee, C. G.; Yasuda, Kenichiro; Inagawa, Jun; Suzuki, Daisuke; et al.

Kaku Busshitsu Kanri Gakkai (INMM) Nihon Shibu Dai-27-Kai Nenji Taikai Rombunshu (CD-ROM), 9 Pages, 2006/00

no abstracts in English

Journal Articles

R&D on safeguards environmental sample analysis at JAERI

Sakurai, Satoshi; Magara, Masaaki; Usuda, Shigekazu; Watanabe, Kazuo; Esaka, Fumitaka; Hirayama, Fumio; Lee, C. G.; Yasuda, Kenichiro; Kono, Nobuaki; Inagawa, Jun; et al.

Proceedings of International Conference on Nuclear Energy System for Future Generation and Global Sustainability (GLOBAL 2005) (CD-ROM), 6 Pages, 2005/10

no abstracts in English

71 (Records 1-20 displayed on this page)