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JAEA Reports

Stable hydrogen and oxygen isotope analyses of geological samples using a thermal conversion elemental analyzer-isotope ratio mass spectrometer at Tono Geoscience Center

Yamamoto, Yusuke*; Watanabe, Takahiro; Niwa, Masakazu; Shimada, Koji

JAEA-Testing 2023-003, 67 Pages, 2024/02

JAEA-Testing-2023-003.pdf:4.63MB

A long-term geosphere stability for geological disposal is evaluated by the past geological environmental changes and modern conditions. Stable hydrogen and oxygen isotope ratios ($$delta$$D, $$delta$$$$^{18}$$O) of geological samples are useful information to estimate the past environmental changes and modern conditions. Recently, the thermal conversion elemental analyzer and isotope ratio mass spectrometer (TC-EA/IRMS) were installed in the Tono Geoscience Center for $$delta$$D and $$delta$$$$^{18}$$O measurements of geological samples. In this study, we reported analytical methods of $$delta$$D and $$delta$$$$^{18}$$O using international standard reference materials. In addition, evaluation tests of uncertainty by repeated analyses of the standards were performed using the TC-EA/IRMS. Furthermore, the $$delta$$D and $$delta$$$$^{18}$$O analyses by the TC- EA/IRMS were also applied to fault rock samples.

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.

JAEA Reports

Proceedings of the 34th Meeting for Tandem Accelerators and their Associated Technologies

Kabumoto, Hiroshi; Nakagawa, Sohei; Matsuda, Makoto

JAEA-Conf 2022-002, 146 Pages, 2023/03

JAEA-Conf-2022-002.pdf:9.89MB

"The 34th Meeting for Tandem Accelerators and their Associated Technologies" was held on July 21-22, 2022 organized by Nuclear Science Research Institute of the Japan Atomic Energy Agency. This meeting was held only on-line for preventing the spread of COVID-19 infection. The purpose of this meeting is contribution of development for related technology and of management of facilities through exchange of information among the researchers and engineers using and operating electrostatics accelerator facilities like tandem accelerators. There were 25 presentations which contains current status report of facility, technical development of accelerator, research of application. The total number of participants was a hundred, from 26 universities, research organizations and industries. This meeting consisted of only oral session, a poster session was not carried out because of on-line meeting. This proceeding compiles the contents of report papers in the meeting.

Journal Articles

Development of an ion funnel reaction cell for suppression of isobaric interference in chrorin-36 dating

Jinno, Satoshi; Fujita, Natsuko; Tanuma, Hajime*

Dai-23-Kai AMS Shimpojiumu Hokokushu, p.89 - 92, 2022/12

The measurement of chlorine-36 ($$^{36}$$Cl) in AMS, which is important for the dating of saline groundwater, is more difficult than other nuclides due to the isobaric interference by sulfur-36 ($$^{36}$$S). In general, acceleration voltages of 6 MV or higher are required to separate $$^{36}$$Cl and $$^{36}$$S. Therefore, this study aims to develop an ion funnel reaction cell and incorporate it into the low energy side of JAEA-AMS-TONO-5MV to selectively suppress $$^{36}$$S.

Journal Articles

Frontiers of studies utilizing accelerator mass spectrometry in geoscience

Honda, Maki

Journal of the Mass Spectrometry Society of Japan, 70(4), p.282 - 283, 2022/12

The development of measurement and chemical separation techniques in the accelerator mass spectrometry (AMS) method has enabled highly sensitive analysis of $$^{244}$$Pu (half-life 8.1$$times$$10$$^{7}$$ years), $$^{60}$$Fe (half-life 2.62$$times$$10$$^{6}$$ years), and $$^{90}$$Sr (half-life 28.9 years) in AMS. For example, the study analyzing $$^{244}$$Pu in ferromanganese crust samples successfully quantified $$^{244}$$Pu from outside the solar system, which had been hidden by $$^{244}$$Pu from nuclear tests. Furthermore, the research has revealed that $$^{244}$$Pu is produced in neutron star mergers, etc., leading to unraveling the production sites where the heavy elements originate. This topic highlights the frontline of studies on $$^{244}$$Pu, $$^{60}$$Fe, and $$^{90}$$Sr utilizing AMS.

Journal Articles

Challenging studies by accelerator mass spectrometry for the development of environmental radiology; Status report on the analysis of $$^{90}$$Sr and $$^{135}$$Cs by AMS

Honda, Maki; Martschini, M.*; Wieser, A.*; Marchhart, O.*; Lachner, J.*; Priller, A.*; Steier, P.*; Golser, R.*; Sakaguchi, Aya*

JAEA-Conf 2022-001, p.85 - 90, 2022/11

Accelerator mass spectrometry (AMS) is an analytical method that combines mass spectrometry with a tandem accelerator, which has been used mainly in nuclear physics experiments. AMS is used to measure radionuclides with half-lives of 10$$^{3}$$-10$$^{8}$$ years. For radionuclides with half-lives of this order, the method of measuring their mass is 10$$^{3}$$-10$$^{6}$$ times more sensitive than measuring their activity. Because of this advantage, AMS has been widely applied in Earth and planetary sciences, atomic energy research, and other fields. Among the various studies, Wallner et al. (2021, 2016) have achieved excellent work in Earth and planetary sciences. For example, they have attained the ultra-sensitive analysis of $$^{60}$$Fe and $$^{244}$$Pu in environmental samples. These are radionuclides produced by rapid-neutron-capture (r-process) nucleosynthesis. Our recent work shows that a new AMS system (VERA, University of Vienna), which combines laser isobaric separation and a typical AMS system, has been successfully applied to the ultra-sensitive determination of $$^{90}$$Sr and $$^{135}$$Cs in environment. For $$^{90}$$Sr in environmental samples, the $$beta$$-ray measurement by the milking of the daughter nuclide $$^{90}$$Y is still the principal method, which takes 3-6 weeks. The new AMS method has a detection limit of $$<$$ 0.1 mBq, which is comparable to that of $$beta$$-ray measurement, with a more straightforward chemical treatment than $$beta$$-measurement. Our achievement demonstrates that AMS can be a practical new method for determining $$^{90}$$Sr in the environment.

Journal Articles

U-Pb dating of calcium carbonate using LA-ICP-MS

Yokoyama, Tatsunori

Isotope News, (764), p.11 - 14, 2019/08

no abstracts in English

Journal Articles

A Spectroscopic technique for analysis developed in the field of unclear energy

Kusaka, Ryoji

Bunko Kenkyu, 67(6), p.239 - 240, 2018/12

A spectroscopic technique for analysis developed by collaboration between Japan Atomic Energy Agency (JAEA) and Quantum and Radiological Science and Technology (QST) is discussed for readers outside the field of nuclear energy. This paper introduces a quantitative analysis for $$^{107}$$Pd radioisotope contained in a spent nuclear fuel by using laser-induced photoreduction and inductively coupled plasma mass spectrometry (ICP-MS). The importance and problems of quantitative analysis for radioisotopes in spent nuclear fuels are described, and the principle, advantages, and future applications of the spectroscopic technique are discussed.

Journal Articles

Effect of surface conditions of the filament used in thermal ionization mass spectrometry on an uranium isotopic measurement

Taguchi, Shigeo; Miyauchi, Hironari*; Horigome, Kazushi; Yamamoto, Masahiko; Kuno, Takehiko

Bunseki Kagaku, 67(11), p.681 - 686, 2018/11

In thermal ionization mass spectrometry, de-gassing is one of the important treatments to release impurities of filaments and to minimize the influence of background. In this work, the effect of the surface change in the tungsten filament induced by the conductively heating treatment on uranium isotopic ($$^{235}$$U/$$^{238}$$U) measurement has been investigated. It was found that the conductively heating treatment of the filament has the effect of smoothing the surface of the filament and also has the effect of improving the deposition of the sample on the filament surface. As a result of either these effects, the precision of uranium isotopic ($$^{235}$$U/$$^{238}$$U) measurement was improved.

Journal Articles

Trace analysis for nuclear non-proliferation and security

Esaka, Fumitaka

Bunseki, 2018(10), p.408 - 411, 2018/10

Recent development of analytical techniques for identification of particles containing nuclear materials, isotope ratio analysis of uranium and plutonium using mass spectrometry, and age determination is described in this paper. These techniques are successfully applied to the trace analysis for nuclear non-proliferation.

Journal Articles

Rapid separation of zirconium using microvolume anion-exchange cartridge for $$^{93}$$Zr determination with isotope dilution ICP-MS

Asai, Shiho; Hanzawa, Yukiko; Konda, Miki; Suzuki, Daisuke; Magara, Masaaki; Kimura, Takaumi; Ishihara, Ryo*; Saito, Kyoichi*; Yamada, Shinsuke*; Hirota, Hideyuki*

Talanta, 185, p.98 - 105, 2018/08

 Times Cited Count:8 Percentile:31.98(Chemistry, Analytical)

Estimating the risks associated with radiation from long-lived fission products (LLFP) in radioactive waste is essential to ensure the long-term safety of potential disposal sites. In this study, the amount of $$^{93}$$Zr, a LLFP, was determined by ICP-MS after separating Zr from a spent nuclear fuel solution using a microvolume anion-exchange cartridge (TEDA cartridge). The TEDA cartridge achieved highly selective separation of Zr regardless of its small bed volume of 0.08 cm$$^{3}$$. The time taken to complete the Zr separation was 1.2 min with a flow rate of 1.5 mL/min, which was 10 times faster than that for a conventional anion-exchange resin column. Almost all the other elements were removed, leading to accurate measurement of $$^{93}$$Zr. The result connects experimental value to theoretical prediction provided by ORIGEN2, which requires verification. With the measured value, we demonstrated that the theoretical value is reliable enough to estimate radiation risks.

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:55.65(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

Uranium age-dating using in-situ isotope ratios by thermal ionization mass spectrometry for nuclear forensics

Okubo, Ayako; Shinohara, Nobuo; Magara, Masaaki

Journal of Radioanalytical and Nuclear Chemistry, 314(1), p.231 - 234, 2017/10

 Times Cited Count:2 Percentile:19.65(Chemistry, Analytical)

The model date of two enriched uranium materials were determined using a new method for nuclear forensics investigation. In this method, the $$^{230}$$Th/$$^{234}$$U ratio was calculated without spike addition from measured ratios of $$^{230}$$Th/$$^{234}$$Th and $$^{234}$$U/$$^{238}$$U, and calculated $$^{234}$$Th/$$^{238}$$U ratio in secular equilibrium. The obtained model date for the low-enriched uranium material was agreed with the known production date within uncertainty. For the highly enriched uranium material, slightly younger model date than the known production date was obtained. The $$^{234}$$U interference on $$^{234}$$Th counting in thermal ionization mass spectrometry measurement was suspected as a potential cause.

Journal Articles

Thermodynamic study of gaseous CsBO$$_{2}$$ by Knudsen effusion mass spectrometry

Nakajima, Kunihisa; Takai, Toshihide; Furukawa, Tomohiro; Osaka, Masahiko

Journal of Nuclear Materials, 491, p.183 - 189, 2017/08

 Times Cited Count:8 Percentile:61.27(Materials Science, Multidisciplinary)

One of the main chemical forms of cesium in the gas phase during severe accidents of light water reactor is expected to be cesium metaborate, CsBO$$_{2}$$, by thermodynamic equilibrium calculation considering reaction with boron. But accuracy of the thermodynamic data of gaseous metaborate, CsBO$$_{2}$$(g), has been judged as poor quality. Thus, Knudsen effusion mass spectrometric measurement of CsBO$$_{2}$$ was carried out to obtain reliable thermodynamic data. The evaluated values of standard enthalpy of formation of CsBO$$_{2}$$(g), $$Delta$$$$_{f}$$H$$^{circ}$$$$_{298}$$(CsBO$$_{2}$$,g), by the 2nd and 3rd law treatments are -700.7$$pm$$10.7 kJ/mol and -697.0$$pm$$10.6 kJ/mol, respectively, and agree with each other within the errors, which suggests our data are reliable. Further, it was found that the existing data of the Gibbs energy function and the standard enthalpy of formation agreed well with the values evaluated in this study, which indicates the existing thermodynamic data are also reliable.

JAEA Reports

Preparation of Zr-91 stable isotope standard solution for determination of Zr-93 by mass spectrometry

Konda, Miki; Asai, Shiho; Hanzawa, Yukiko; Magara, Masaaki

JAEA-Technology 2015-054, 22 Pages, 2016/03

JAEA-Technology-2015-054.pdf:3.44MB

Isotope dilution mass spectrometry (IDMS) with ICP-MS is reliable method for determination of Zr-93, which is one of the long-lived fission products found in spent nuclear fuel and high-level radioactive wastes. In order to use an isotope standard solution of zirconium as the spike for IDMS, dissolving a commercially available solid isotope standard is indispensable. Prior to the dissolution of the Zr-91 isotope standard, solubility of metal zirconium in a mixture of HNO$$_3$$ and HF was evaluated using zirconium metal chips. Then, 2 mg of the Zr-91 isotope standard was dissolved with 0.2 mL of 1 M HNO$$_3$$-3 v/v% HF mixed solution, followed by adjusting the concentration of Zr-91 to approximately 1,000 $$mu$$g/g. IDMS, in which a natural isotopic abundance standard solution of zirconium was used as the spike, was employed for the determination of the concentration of Zr-91 in the prepared Zr-91 isotope standard solution. The concentration of Zr-91 in the prepared Zr-91 isotope standard solution was (9.6$$pm$$1.0) $$times$$ 10$$^2$$ $$mu$$g/g, which is in good agreement with the predicted concentration. This indicates that the Zr-91 metal isotope standard was completely dissolved with sufficient chemical stability. Additionally, no impurities were detected in the prepared Zr-91 isotope standard solution. These positive results denote that the Zr-91 isotope standard solution with the preferable quality for IDMS of Zr-93 can be obtained by the proposed dissolution procedures.

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

New wind into the Atomic Collision Society of Japan

Matsubara, Akihiro

Shototsu, 12(4), P. 126, 2015/07

no abstracts in English

Journal Articles

Identifying uranium particles using fission tracks and microsampling individual particles for analysis using thermal ionization mass spectrometry

Esaka, Fumitaka; Suzuki, Daisuke; Magara, Masaaki

Analytical Chemistry, 87(5), p.3107 - 3113, 2015/03

 Times Cited Count:13 Percentile:44.45(Chemistry, Analytical)

The analysis of uranium particles in environmental samples taken from nuclear facilities is a useful tool to unveil undeclared nuclear activities related to the production of nuclear weapons. An efficient method to analyze isotope ratios of individual uranium particles is thermal ionization mass spectrometry (TIMS) combined with a fission track technique. A drawback in the fission track-TIMS technique is so-called particle-mixing. Here, some uranium particles are measured as a single particle and an averaged isotope ratio is obtained, which may lead to misunderstanding conclusions for source identification. In the present study, micro-sampling under a scanning electron microscope has been added to the procedure of the fission track-TIMS technique. The analysis of a mixed sample containing uranium particles in SRM 950a and CRM U100 materials indicated that the problem of particle mixing was almost avoidable with the proposed technique.

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:26.85(Physics, Applied)

Journal Articles

Determination of $$^{129}$$I in environmental samples by AMS and NAA using an anion exchange resin disk

Suzuki, Takashi; Bamba, Shigeru*; Kitamura, Toshikatsu; Kabuto, Shoji*; Isogai, Keisuke*; Amano, Hikaru

Nuclear Instruments and Methods in Physics Research B, 259(1), p.370 - 373, 2007/06

 Times Cited Count:14 Percentile:68.37(Instruments & Instrumentation)

no abstracts in English

201 (Records 1-20 displayed on this page)