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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

Chemical state and isotope ratio analysis of individual uranium particles by a combination of micro-Raman spectroscopy and secondary ion mass spectrometry

Yomogida, Takumi; Esaka, Fumitaka; Magara, Masaaki

Analytical Methods, 9(44), p.6261 - 6266, 2017/11

 Times Cited Count:9 Percentile:55.41(Chemistry, Analytical)

A combination of micro-sampling, micro-Raman spectroscopy (MRS), and secondary ion mass spectrometry (SIMS) was applied to the characterization of individual uranium particles. Reference particles with U$$_{3}$$O$$_{8}$$ (NBL CRM U010) and UO$$_{2}$$ were identified by scanning electron microscopy combined with energy dispersive X-ray detection (SEM-EDX) and transferred onto grassy carbon substrates by micro-sampling. The crystalline phases of the reference particles with diameters ranging from 1 $$mu$$m to 5 $$mu$$m were determined non-destructively by using MRS thanks to the optimization of laser power at the measurement. Isotope ratios were also determined with SIMS after the MRS analysis and were consistent with values in the literature. These results indicate that chemical forms and isotope ratios of individual uranium particles as small as 1 $$mu$$m can be analyzed efficiently by using the proposed method.

Journal Articles

Surface analysis

Esaka, Fumitaka

Ekisupato Oyo Kagaku Sirizu; Kiki Bunseki, p.119 - 135, 2015/09

Bulk analysis has been conventionally used for measuring solid materials. In contrast, surface analysis is extensively used for analyzing chemical compositions and chemical states of solid surface. The surface compositions often differ from those of bulk materials. Recently, doping of impurity elements and deposition of thin films on the surface of the materials are key techniques to fabricate functional materials. Therefore, surface analysis becomes important to characterize such materials. In this paper, the principle and feature of some surface analytical techniques are described.

Journal Articles

Transmission secondary ion mass spectrometry using 5 MeV C$$_{60}$$$$^{+}$$ ions

Nakajima, Kaoru*; Nagano, Kengo*; Suzuki, Motofumi*; Narumi, Kazumasa; Saito, Yuichi; Hirata, Koichi*; Kimura, Kenji*

Applied Physics Letters, 104(11), p.114103_1 - 114103_4, 2014/03

 Times Cited Count:6 Percentile:26.7(Physics, Applied)

Journal Articles

Application of secondary ion mass spectrometry to the measurement of lead isotope ratio in individual particles

Esaka, Fumitaka; Watanabe, Kazuo; Magara, Masaaki; Usuda, Shigekazu

Instrumentation Science & Technology, 32(2), p.103 - 114, 2004/03

The capability of secondary ion mass spectrometry (SIMS) for lead isotope ratio measurements of individual particles has been demonstrated by measuring lead-containing particles in three kinds of environmental certified reference materials (CRMs): urban particulate matter, vehicle exhaust particulates and coal fly ash. The isotope ratios of $$^{207}$$Pb/$$^{206}$$Pb and $$^{208}$$Pb/$$^{206}$$Pb for the individual particles on the carrier were determined by SIMS. The relative standard deviations of the lead isotope ratios were less than 1.6 % for all particles measured. It was demonstrated that the results of the lead isotope ratios were clearly distinguished among the three samples. Moreover, the particles in the vehicle exhaust particulate sample were classified into two groups according to lead isotope ratios. The results indicated that the present SIMS technique can provide detailed information with regard to the origin and the transportation of individual particles.

Journal Articles

Isotope ratio analysis of individual uranium particles for safeguards

Esaka, Fumitaka; Watanabe, Kazuo; Fukuyama, Hiroyasu; Onodera, Takashi; Esaka, Konomi; Inagawa, Jun; Iguchi, Kazunari; Suzuki, Daisuke; Lee, C. G.; Magara, Masaaki; et al.

Dai-25-Kai Kaku Busshitsu Kanri Gakkai Nihon Shibu Nenji Taikai Rombunshu, p.128 - 135, 2004/00

Japan Atomic Energy Research Institute (JAERI) was qualified as a member of the IAEA network analytical laboratories (NWALs) for particle and bulk analyses of safeguards environmental samples in January 2003. The particle analysis gives more detailed information on nuclear facility operation than the bulk analysis because the isotope ratios of nuclear materials in the samples collected inside nuclear facilities (swipe samples) can be determined for individual particles. We applied, as a method for uranium isotope ratio measurement, secondary ion mass spectrometry (SIMS) to particle analysis. Prior to the SIMS analysis, the particles in a swipe sample are recovered onto a carrier by impaction. The carriers with the recovered particles are then screened by total reflection X-ray fluorescence spectrometry. We integrated these techniques into a standard procedure, which is applied to domestic and IAEA swipe samples routinely.

Journal Articles

Isotope ratio analysis of individual particles containing nuclear materials in safeguards environmental samples

Esaka, Fumitaka

Bunseki, 2003(11), p.688 - 691, 2003/11

Isotope ratio measurement for individual particles containing uranium in swipe samples taken at nuclear facilities is a powerful tool to verify the absence of undeclared nuclear activities. In order to develop the analysis technique, we have investigated a series of methods: particle recovery from the swipe sample, particle screening and isotope ratio analysis for individual particles. As the result, the 235U/238U ratio was determined with the relative standard deviation within 2.0 % for the particle with a diameter of 1 um.

Journal Articles

Strongly enhanced secondary ion emission by molecular ion irradiation

Yamamoto, Hiroyuki; Saito, Takeru; Asaoka, Hidehito

Journal of Trace and Microprobe Techniques, 19(4), p.571 - 579, 2001/11

 Times Cited Count:4 Percentile:14.99(Chemistry, Analytical)

no abstracts in English

Journal Articles

Silicon cluster formation by molecular ion irradiation; Relationship between iradiated ion species and cluster yield

Yamamoto, Hiroyuki; Saito, Takeru; Asaoka, Hidehito

Applied Surface Science, 178(1-4), p.127 - 133, 2001/07

 Times Cited Count:5 Percentile:32.75(Chemistry, Physical)

no abstracts in English

Journal Articles

Application of SIMS and TXRF techniques to lead air-pollution monitoring

Esaka, Fumitaka; Zheng, W.*; Watanabe, Kazuo; Magara, Masaaki; Hanzawa, Yukiko; Usuda, Shigekazu; Adachi, Takeo

Advances in Mass Spectrometry, 15, p.973 - 974, 2001/00

no abstracts in English

Journal Articles

Development and application of PIE apparatuses for high-burnup LWR fuels

; Mita, Naoaki; Nishino, Yasuharu; Amano, Hidetoshi

JAERI-Conf 99-009, p.103 - 111, 1999/09

no abstracts in English

Journal Articles

Emission of silicon cluster ions by molecular ion bombardment

Yamamoto, Hiroyuki; Baba, Yuji

Applied Physics Letters, 72(19), p.2406 - 2408, 1998/05

 Times Cited Count:9 Percentile:42.99(Physics, Applied)

no abstracts in English

JAEA Reports

None

Sonobe, Hitoshi; Ishiguro, Katsuhiko

PNC TN8410 92-114, 85 Pages, 1992/03

PNC-TN8410-92-114.pdf:4.03MB

None

Oral presentation

Transmission secondary ion mass spectrometry of phenylalanine on silicon nitride membranes using MeV monoatomic and cluster ions

Nakajima, Kaoru*; Nagano, Kengo*; Suzuki, Motofumi*; Narumi, Kazumasa; Saito, Yuichi; Hirata, Koichi*; Kimura, Kenji*

no journal, , 

Oral presentation

Isotopic analysis of uranium particles in environmental samples with SIMS

Esaka, Fumitaka

no journal, , 

We are developing particle analysis techniques using secondary ion mass spectrometry for safeguards swipe samples. Isotope ratios of individual uranium particles in the samples taken at nuclear facilities are measured to unveil undeclared nuclear activities. For this purpose, fission track and alpha track techniques are utilized to identify uranium particles and SIMS is used for isotope ratio analysis.

Oral presentation

Transmission secondary ions mass spectrometry of an amino acid using 5 MeV C$$_{60}$$ ions

Nakajima, Kaoru*; Nagano, Kengo*; Suzuki, Motofumi*; Narumi, Kazumasa; Saito, Yuichi; Hirata, Koichi*; Kimura, Kenji*

no journal, , 

no abstracts in English

Oral presentation

Forward emission of secondary ions from amino acids and peptides films on SiN membranes penetrated by swift C$$_{60}$$$$^{+}$$ from the backside

Marumo, Tomoya*; Nakajima, Kaoru*; Kimura, Kenji*; Narumi, Kazumasa; Saito, Yuichi

no journal, , 

no abstracts in English

Oral presentation

Secondary ion mass spectrometry combined with micro-Raman spectroscopy for isotopic and chemical analysis of individual uranium particles

Yomogida, Takumi; Esaka, Fumitaka; Magara, Masaaki

no journal, , 

Analysis of individual uranium particles in environmental samples from nuclear facilities is useful for detecting nuclear activity. Uranium isotope ratios in the samples are measured to detect nuclear activities related to production of nuclear weapons. We can detect the nuclear activities such as refining, conversion and enrichment process by determination of the chemical form of uranium particles. In this study, we developed a secondary ion mass spectrometry combined with micro-Raman spectroscopy for isotopic and chemical analysis of individual uranium particles. The developed methods have been applied to the analysis of reference uranium materials. As a result, the isotope ratios and the chemical form of individual uranium particle can be analyzed with the proposed method.

Oral presentation

Development of pretreatment and analysis for environmental samples containing radiocaesium; Preliminary ToF-SIMS analysis of Cs isotope ratio in the microparticle

Tagomori, Hisaya*; Kawamura, Hidehisa*; Kusano, keiichi*; Dohi, Terumi

no journal, , 

To investigate their spatial distribution and physicochemical properties of the radiocaesium-bearing micro particles (CsMPs), an efficient methodology for determine and analysis them is required. Here we focused on CsMPs from litters as they may affect the radiocaesium cycling in forest ecosystem. In this study we developed a method to determine CsMPs (mostly 1-10 $$mu$$m sizes) from litters by combine digestion treatment and automatic particle analysis with FE-EPMA. In total it took up to 3 days for detecting one CsMP from huge amounts of mineral-like and metallic particles. In the ToF-SIMS analysis for Cs isotope ratios of CsMPs to understand their emission source as the next step, pretreatment for easily detecting micron-sized samples is needed. To solve this problem, FIB technique was used for Gallium marking formation around target sample. Preliminary Cs isotope ratios(133Cs, 134(Cs + Ba), 135Cs, 137(Cs + Ba)) and their distributions of CsMPs were determined by applying these approaches. We developed pretreatment for microscopy and ToF-SIMS analysis of CsMPs.

Oral presentation

Utilization of Secondary mass spectrometry (SIMS) in nuclear-related fields; Isotopic composition analysis of micron sized nuclear particles for nuclear safeguards

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

no journal, , 

We are applying a secondary ion mass spectrometer (SIMS) to measure the isotopic composition of micron-sized nuclear particles in environmental samples for safeguards purposes. International Atomic Energy Agency (IAEA) collects swipe samples taken from the walls and floors of nuclear facilities through on-site inspections, and analyzes uranium isotopic composition of these samples for confirming the absence of undeclared nuclear activity. As a member of IAEA network analytical laboratories (NWALs), our research group has not only reported the analytical results of isotopic composition of U and Pu in the inspection samples to IAEA, but also has been developed analytical techniques to precisely and accurately measure the isotopic composition of nuclear materials on the IAEA swipe samples. Our analytical activity at Clean Laboratory for Environmental Analysis and Research (CLEAR) in JAEA, and analytical techniques using SIMS are introduced.

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