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Journal Articles

Improvement in automated particle measurement using micromanipulation and large geometry secondary ion mass spectrometry to remove the particle mixing effect of uranium particles

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

Journal of Nuclear Science and Technology, 10 Pages, 2025/05

A new automated particle measurement (APM) combined with micromanipulation using large geometry secondary ion mass spectrometry instrument was proposed and demonstrated to remove the particle mixing effect, which indicated that the aggregation of uranium particles was detected as a single uranium particle, from APM results. The results showed that the new APM method was more effective than the traditional APM method in removing the particle mixing effect from the APM results and determining the existence of minor uranium isotopes in the samples.

Journal Articles

Sensitive $$^{236}$$U/$$^{238}$$U isotopic analysis of trace uranium in safeguards environmental samples using multicollector inductively coupled plasma mass spectrometry

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

Journal of the American Society for Mass Spectrometry, 35(6), p.1178 - 1183, 2024/05

 Times Cited Count:0 Percentile:0.00(Biochemical Research Methods)

A sensitive analytical technique was investigated in order to determine 10$$^{-7}$$ order of $$^{236}$$U/$$^{238}$$U ratio in the sub-ng of uranium using a multi-collector ICP-MS. First, the solution volume was concentrated to one tenth to obtain higher intensities. Next, data acquisition was started from the beginning of the solution uptake and continued until all solution was exhausted. Taking advantage of multi-collector measurement, all data were used with excepting the portion affected by air mixing at the beginning and end of sample introduction. The isotope ratios were calculated from the total counts of each isotope. This technique was applied to U isotope standard (IRMM-184) to measure the 10$$^{-7}$$ order of $$^{236}$$U/$$^{238}$$U ratio in the sub-ng of uranium. Measured values were in good agreement with the certified value within the uncertainity ($$k$$=2). The uncertainties obtained with this new technique (32% on average) were revised to be 10 times smaller than those obtained with the conventionalmethod.

Journal Articles

Assessment of caesium-137 detections at CTBTO radionuclide monitoring stations in East Asia and their relationship to Asian dust dispersion

Furuno, Akiko; Omori, Ryuta*; Tateoka, Hisanori*; Minakawa, Yuya*; Kurihara, Toshiyuki; Yamamoto, Yoichi; Tomita, Yutaka

Pure and Applied Geophysics, 14 Pages, 2024/00

 Times Cited Count:0 Percentile:0.00(Geochemistry & Geophysics)

The Comprehensive Nuclear-Test-Ban Treaty Organization (CTBTO) Okinawa radionuclide monitoring station (JPP37) is located on a hill facing the East China Sea at the center of the main island of Okinawa. It occasionally detects Cs-137, although no nuclear facilities are located on the island. This study focused on the detection of Cs-137 at JPP37 and examined the ratio of simultaneous detections at nearby stations of the International Monitoring System (IMS) of the CTBTO and the relationship with Asian dust from inland East Asia. The detection of Cs-137 in JPP37 from 2020 to 2023, which motivated this study, was high in spring. Among the nine IMS radionuclide stations in East Asia, the detections in Beijing, Lanzhou, and Ulaanbaatar, Mongolia, were also high in spring. This suggested a high association with the detection of Asian dust in East Asia. Thus, we confirmed the detection of Cs-137 at nine nearby IMS stations when Asian dust was observed at any of the sites in Japan. In addition, we observed that the detection rates were high in Takasaki, Beijing, Lanzhou, and Ulaanbaatar. It can be inferred that the Cs-137 observed mainly in spring at the IMS particulate radionuclide stations in the East Asian region around Japan were likely to pick up the effects of global fallout conveyed by Asian dust. Thereafter, we conducted a preliminary source estimation analysis for Asian dust arrival near Japan. Atmospheric dispersion simulations explained the detection of Cs-137 at nearby IMS particulate radionuclide stations, assuming that Cs-137 was emitted from the desert, the source of the Asian dust.

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

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

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

An Examination of rapid analysis of $$^{226}$$Ra in natural water samples by ICP-MS

Tomita, Jumpei; Ozawa, Mayumi; Ohara, Yoshiyuki; Miyamoto, Yutaka

KEK Proceedings 2021-2, p.130 - 134, 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:5 Percentile:49.08(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

Development of a resonant laser ionization gas cell for high-energy, short-lived nuclei

Sonoda, Tetsu*; Wada, Michiharu*; Tomita, Hideki*; Sakamoto, Chika*; Takatsuka, Takaaki*; Furukawa, Takeshi*; Iimura, Hideki; Ito, Yuta*; Kubo, Toshiyuki*; Matsuo, Yukari*; et al.

Nuclear Instruments and Methods in Physics Research B, 295, p.1 - 10, 2013/01

 Times Cited Count:21 Percentile:81.61(Instruments & Instrumentation)

no abstracts in English

JAEA Reports

Development of fuel microspheres fabrication by the external gelation process

Tomita, Yutaka; Morihira, Masayuki; Tamaki, Yoshihisa*; Nishimura, Kazuhisa*; Shoji, Shuichi*; Kihara, Yoshiyuki; Kase, Takeshi; Koizumi, Tsutomu

JAEA-Research 2006-088, 95 Pages, 2007/01

JAEA-Research-2006-088.pdf:23.02MB

JAEA has developed sphere-pac fuels in the feasibility study on commercialized FBR cycle systems as one of the candidates for low decontamination TRU fuels. Optimization of the fabrication condition for coarse spheres, development of an improved external gelation process, and examination of peculiar problems for the low decontamination fuel were carried out in Phase II. The results are shown as follows. (1) Fabrication condition of coarse spheres was optimized. (2) Feasibility of the improved external gelation process was confirmed. (3) Rare earth elements did not bring any problem for the characteristic of spheres and fabrication condition. (4) Radiation resistant data of the feed solution was acquired. Results of tests show the feasibility of the external gelation process for the low decontamination TRU fuel microsphere fabrication.

Journal Articles

Fuel microsphere fabrication tests for sphere-pac fuel by the external gelation process

Tomita, Yutaka; Morihira, Masayuki; Kihara, Yoshiyuki; Tamaki, Yoshihisa*

Proceedings of International Conference on Nuclear Energy System for Future Generation and Global Sustainability (GLOBAL 2005) (CD-ROM), 4 Pages, 2005/10

High economic competitiveness and low environmental impact are required for advanced FBR cycle systems. Sphere-pac fuel has been considered as promising fuel systems, due to its inherent advantage in remote operation, dustfree fuel fabrication process and cost reduction. Japan Nuclear Cycle Development Institute (JNC) has been investigated the external gelation process for sphere-pac fuel. In this report, the result of the sphere fabrication test by the external gelation process is reported.

Journal Articles

Fabrication of Sphere-pac Fuel and Vipac Fuel for Irradiation Tests (Collaboration Project among JNC, PSI and NRG)

Tomita, Yutaka; Shigetome, Yoshiaki; Kihara, Yoshiyuki

Saikuru Kiko Giho, (24), p.1 - 10, 2004/00

JNC has carried out the joint research project with PSI in Switzerland and NRG in Netherlands.In this project, three types of fuel segments (sphere-pac segments, vipac segments and pellet segments) were fabricated by PSI. They have been irradiated under same irradiation condition to compare their performances in the High Flux Reactor. This report describes the fabrication of sphere-pac segments and vipac segments for irradiation tests.

Oral presentation

Japan Atomic Energy Agency's efforts to the CTBT verification regime

Yamamoto, Yoichi; Kijima, Yuichi; Tomita, Yutaka

no journal, , 

As a member of the CTBT National Operation System of Japan (NOSJ), JAEA monitors and evaluates radionuclides derived from nuclear tests. For this purpose, Takasaki and Okinawa radionuclide stations, Tokai radionuclide laboratory, and a national data center already were put in place and have been operated. This presentation introduces outline of NOSJ and each facility, the response to a nuclear test event, JAEA's recent activities etc.

Oral presentation

JAEA's recent activities related to CTBT verification regime

Yamamoto, Yoichi; Kijima, Yuichi; Tomita, Yutaka

no journal, , 

This presentation summarizes JAEA's recent activities related to CTBT verification regime. To establish the global verification regime of CTBT for the nuclear tests, JAEA has been operating provisionally three facilities (two monitoring stations and one radionuclide laboratory) of the CTBT international monitoring system and a national data center for radionuclide monitoring. For the 6th nuclear test conducted by North Korea in September 2017, JAEA reported the analysis and evaluation results of data observed at the CTBT radionuclide monitoring stations to the national government etc. in a timely manner and thereby contributed to the evaluation by the national government based on the CTBT operation system in Japan. For the purpose of strengthening CTBTO's detection capability for nuclear tests, JAEA started new noble gas joint measurement project with CTBTO in Horonobe (Hokkaido) and Mutsu (Aomori) based on the Japanese government contribution in 2017.

Oral presentation

Observation results of the Fukushima Daiichi accident at CTBT radionuclide monitoring stations

Yamamoto, Yoichi; Kijima, Yuichi; Tomita, Yutaka

no journal, , 

After the Great East Japan Earthquake in 2011, the Fukushima Daiichi Nuclear Power Plant accident happened and large amounts of radioactive materials were released into the environment and spread globally. The National Data Center-2 (NDC-2) in the Japan Atomic Energy Agency received observation data every day sent from the radionuclide monitoring network of the CTBT International Monitoring System and analyzed the data. The radionuclides released by the accident generally circulated around the northern hemisphere in about 12 days. The activity concentration of Xenon-133 around each radionuclide station in the northern hemisphere almost became uniformed by diffusion in early April, 2011, and after that, the activity concentration at each station decreased with the half-life of Xe-133 and returned to the normal level before the accident in early June. NDC-2 also estimated the timing of first arrival of the radioactive plume at the CTBT Takasaki radionuclide station using the observation data of the station. Consistent results were found between the estimated timing and the time when the spatial gamma-ray dose rate at the monitoring post neat the station rose suddenly.

Oral presentation

Detailed analysis of individual uranium particles in environmental sample by SIMS and pre-screening measurement introduced into the analysis procedure

Tomita, Ryohei; Esaka, Fumitaka; Miyamoto, Yutaka

no journal, , 

In the previous study, we developed a combination method of individual uranium particle manipulation in scanning electron microscope (SEM) and secondary ion mass spectrometry (SIMS) for removing the interferences from other elements in other particles. Since the particles were selected randomly and manipulated, it caused the problem not to cover the range of $$^{235}$$U/$$^{238}$$U isotope ratio in the sample. In this study, we introduced pre-screening measurement into the procedure of analyzing uranium isotope ratios in individual particles by SIMS to cover the range of $$^{235}$$U/$$^{238}$$U in the sample.

Oral presentation

Chemical state analysis of individual uranium particles with electron backscatter diffraction

Esaka, Fumitaka; Yomogida, Takumi; Tomita, Ryohei; Miyamoto, Yutaka

no journal, , 

Chemical state analysis is important to elucidate the origin of particles and its effect on the environment. However, the analysis is difficult because the amounts of elements in individual particles are considerably small. In the present study, electron backscatter diffraction (EBSD) is applied to the chemical state analysis of individual uranium particles. As a result, uranium particles with diameters of 1$$mu$$m were able to be measured and clear electron backscatter patterns were observed. In addition, the patterns of UO$$_{2}$$ particles were distinguished from those of U$$_{3}$$O$$_{8}$$ particles.

Oral presentation

Status report on Japanese NDC-2; Current status of Xenon joint measurement project at Horonobe and Mutsu

Yamamoto, Yoichi; Kijima, Yuichi; Tomita, Yutaka

no journal, , 

Based on repeated DPRK's nuclear tests, the Japanese government contributed funds for the noble gas measurement project in February 2017 for the purpose of strengthening CTBTO's detection capability for nuclear tests. The CTBTO decided to conduct measurements in Hokkaido and Tohoku regions of Japan for the time being, and to enhance JAEA with experiences and performance of measurements in Japan as the responsible organization. In response to this, the JAEA has installed two mobile noble gas measurement systems at Horonobe, Hokkaido and JAEA Ohminato site in Mutsu, Aomori, and been carrying out the joint measurement project with the CTBTO. The current status of this project will be presented.

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