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Analytical method for the determination of $$^{211}$$At using an $$alpha$$-scintillation-camera system and thin-layer chromatography

瀬川 麻里子; 西中 一朗*; 藤 暢輔; 前田 亮

Journal of Radioanalytical and Nuclear Chemistry, 326(1), p.773 - 778, 2020/10

 被引用回数:0 パーセンタイル:100(Chemistry, Analytical)

$$^{211}$$At is a candidate nuclide for alpha-targeted therapy. In order to use $$^{211}$$At as a pharmaceutical, the radioactivity and chemical forms of generated $$^{211}$$At are the most fundamental specifications that need to be analyzed prior to its medical use. However, previous methods of separately measuring the radioactivity and chemical forms are not adaptable to the medical use of $$^{211}$$At because they cause a severe loss of $$^{211}$$At and do not analyze all the chemical forms of $$^{211}$$At. Therefore, a new analytical method for both the radioactivity and chemical forms of generated $$^{211}$$At is urgently needed. Accordingly, in this study, we developed an experimental system optimized to simultaneously analyze both the radioactivity and chemical forms of a $$^{211}$$At solution to significantly shorten the analysis time; we experimentally verified the accuracy and capabilities of this system at the Japan Atomic Energy Agency. The experiments confirmed that the present system could analyze the radioactivity and all the chemical forms of $$^{211}$$At with an uncertainty of approximately 5% in the region higher than 150 Bq and that it was 200 times more sensitive than the conventional method using an imaging technique with an X-ray imaging plate. As a result, a new method for analyzing the radioactivity and chemical forms of $$^{211}$$At was successfully established and this method will meet the demands for alpha-targeted therapy using $$^{211}$$At. This method will contribute to promoting the stable supply of the medical use of $$^{211}$$At in the near future.


Study of shields against D-T neutrons for Prompt Gamma-ray Analysis apparatus in Active-N

古高 和禎; 藤 暢輔

Proceedings of Joint International Conference on Supercomputing in Nuclear Applications + Monte Carlo 2020 (SNA + MC 2020), p.297 - 304, 2020/10

No established method exists to non-destructively measure the amount of highly radioactive nuclear fuel materials such as spent fuels, and it is one of the urgent issues in nuclear material accountancy. Therefore, JAEA has started a research on development of innovative non-destructive analysis (NDA) system for Special Nuclear Materials and Minor Actinides, in cooperation with EC-JRC. The aim of the project is to establish an NDA method which can be applied to highly radioactive nuclear materials and develop a demonstration system, named "Active-N", by utilizing an intense D-T neutron source and by combining the following mutually complemental active-neutron NDA methods: DDA, N RTAs, and PGA (Prompt Gamma-ray Analysis). The PGA measurements play a crucial role in the system, because it can detect/quantify neutron poison elements which disturb DDA measurements, as well as explosives and chemical warfare agents, by utilizing a high-energy resolution Germanium detector. To make an NDA system to be efficient one, an intense neutron generator has to be employed. On the other hand, exposure of a Ge detector to an immense amount of fast neutron makes the detector severely damaged and inoperative. Therefore, in order for the system to be efficient, it is essential to develop effective shield of the PGA system against fast neutrons. In this work, by performing particle transport calculation using Monte Carlo method, we have investigated effective shielding methods for the PGA measurement system in the Active-N system, against fast neutrons from the D-T neutron source. Materials and their configurations which effectively reduce fast-neutron doses and at the same time emit no interfering gamma rays, were examined. Through the calculation, a shield which reduces fast neutron dose sufficiently have been developed. This research was implemented under the subsidiary for nuclear security promotion of MEXT.


Study of the Li($$d,xn$$) reaction for the development of accelerator-based neutron sources

渡辺 幸信*; 定松 大樹*; 荒木 祥平*; 中野 敬太*; 川瀬 頌一郎*; 金 政浩*; 岩元 洋介; 佐藤 大樹; 萩原 雅之*; 八島 浩*; et al.

EPJ Web of Conferences, 239, p.20012_1 - 20012_4, 2020/09

重陽子ビームによる加速器中性子源は、核分裂生成物の核変換、核融合炉材料試験等の応用分野での利用が検討されている。そこで、このような加速器や中性子源の設計に有益なデータとして、大阪大学核物理研究センターにおいて、200MeV重陽子入射核反応によるリチウムの中性子生成二重微分断面積(DDX)を測定した。実験では液体有機シンチレータEJ301を用いた飛行時間法を適用し、前方0度から25度の範囲で中性子断面積データを取得した。広範なエネルギー範囲のデータを取得するため、直径及び厚さが5.08cmと12.7cmの大きさの異なる2台のシンチレータを標的から7mと20mの地点にそれぞれ設置した。ここで、中性子の検出効率はSCINFUL-QMDコードを用いて導出した。本発表では、実験値と重陽子入射断面積計算コードDEURACS及び粒子・重イオン輸送計算コードPHITSによる計算値との比較について述べる。また、25, 40及び100MeV重陽子入射による実験値を用いて、DDXの入射エネルギー依存性について議論する。


Improvement of detection limit in differential die-away analysis system for nuclear non-proliferation and nuclear security

大図 章; 前田 亮; 米田 政夫; 藤 暢輔

Proceedings of 2019 IEEE Nuclear Science Symposium and Medical Imaging Conference (IEEE NSS/MIC 2019), Vol.1, p.101 - 104, 2020/08

In the fields of safeguards, nuclear non-proliferation, and nuclear security, non-destructive analysis (NDA) techniques useful for highly radioactive nuclear materials (NMs) are not established yet because there are so many technical difficulties to measure the amount of the highly radioactive NMs. A novel NDA system with a pulsed neutron source as the method for determining the composition of mixed NMs has been developing in the Japan Atomic Energy Agency. In the NDA system, a differential die-away analysis (DDA) technique is used to quantify the amount of fissile materials. The detection limit of fissile materials in DDA system is determined by the signal to noise ratio in fast neutron counting. A method to reduce the noise signal by using neutron absorber (B$$_{4}$$C rubber) sheets mounted on the inner entire surface in the sample cavity is proposed. The effect of the sheets on the reduction of noise signal in the fast neutron counting was investigated in both experimental test and simulation. The experimental results show that it is possible to detect a nuclear fissile material ($$^{239}$$Pu) of as low as 1 mg in a vial bottle when the absorber sheets with a thickness of 3 mm is used. This paper also presents comparison between experimental data and simulation results.


Measurement of defect-induced electrical resistivity change of tungsten wire at cryogenic temperature using high-energy proton irradiation

岩元 洋介; 吉田 誠*; 松田 洋樹; 明午 伸一郎; 佐藤 大樹; 八島 浩*; 薮内 敦*; 木野村 淳*; 嶋 達志*

JPS Conference Proceedings (Internet), 28, p.061003_1 - 061003_5, 2020/02



Conceptual study on a novel method for detecting nuclear material using a neutron source

米田 政夫; 藤 暢輔

Annals of Nuclear Energy, 135, p.106993_1 - 106993_6, 2020/01

 被引用回数:0 パーセンタイル:100(Nuclear Science & Technology)



Development of active neutron NDA system

藤 暢輔

JAEA-Conf 2019-001, p.47 - 52, 2019/11

原子力機構と欧州委員会-共同研究センター(EC-JRC)との共同研究により、従来の非破壊測定技術が適用できない高線量核燃料物質のための非破壊測定技術開発を実施している。本プロジェクトでは、小型のパルス中性子源を用いる4つのアクティブ中性子法(ダイアウェイ時間差分析法: DDA、中性子共鳴透過分析法: NRTA、即発$$gamma$$線分析法: PGA、遅発$$gamma$$線分析法: DGA)の開発を実施しており、それらの手法を組み合わせ、それぞれの特長を生かすことによって高線量核燃料物質に対応できる非破壊測定法の確立を目指している。平成29年度で終了したフェーズIに続き、平成30年度から開始したフェーズIIでは、上述の4つのアクティブ中性子法の高度化を行うとともに、原子力機構燃料サイクル安全工学研究施設において、3つの分析手法(DDA, PGA, NRTA)を組み合わせた総合非破壊測定装置を開発する予定である。本講演では、プロジェクトの概要とこれまでに得られた主な研究成果について報告する。本研究開発は、文部科学省「核セキュリティ強化等推進事業費補助金」事業の一部である。


Performance evaluation of differential die-away system in an integrated active neutron NDA system for nuclear non-proliferation and nuclear security

大図 章; 前田 亮; 米田 政夫; 藤 暢輔

Proceedings of 2018 IEEE Nuclear Science Symposium and Medical Imaging Conference (IEEE NSS/MIC 2018) (Internet), 4 Pages, 2019/10

A Differential Die-away Analysis (DDA) system using a compact pulsed neutron (DT: 14 MeV) generator has been successfully developed for nuclear non-proliferation and nuclear security in the Japan Atomic Energy Agency. The DDA system employing the fast neutron direct interrogation method is designed to quantify fissile materials in samples which have different volume from a vial bottle (4 cc) to pail container (20 liter). It has been demonstrated experimentally that the DDA system is capable of quantifying a nuclear fissile material (Pu-239) less than 10 mg in a vial bottle. The performance of the DDA system with a large measurement sample such as a MOX can container (2 liter) was evaluated through the Monte Carlo simulation studies. The simulation results show that the Pu-239 mass of around 10 mg even in the MOX can container can be detected. The results of the simulation study are discussed and compared to those of the experimental test.



佐藤 大樹; 岩元 洋介; 小川 達彦

2017年度量子科学技術研究開発機構施設共用実施報告書(インターネット), 1 Pages, 2019/08

数10MeV以上のエネルギー領域での陽子入射反応における前方方向の中性子生成に関して、理論模型および核データともに実験データの不足から予測精度の検証が十分になされていない。本研究では、原子力機構が開発している汎用放射線輸送計算コードPHITSの精度向上に資するため、最前方方向(入射軸に対して0$$^{circ}$$方向)の中性子生成二重微分断面積の系統的な実験データ整備を進めている。平成28年度までに20, 34, 48, 63および78MeV陽子入射の測定を実施したが、絶対値に関する精度改善のため34MeV陽子入射に対しては、より薄い標的を採用して再測定した。実験では、量子科学技術研究開発機構高崎量子応用研究所TIARAのAVFサイクロトロンから供給される陽子ビームをC, Al, FeおよびPb標的に入射し、生成中性子を最前方方向に開いたコリメータを通して測定室に導き、シンチレーション検出器で測定した。また、PHITSでは、核内カスケード模型に基づくINCLおよび評価済み核データライブラリJENDL-4.0/HEにより、中性子生成の計算を行った。実験値と計算値との比較から、INCLはすべての反応に対して実験値よりも大きな値を与え、JENDL-4.0/HEはFeの結果を良好に再現するが、Alに対しては過大評価し、Pbに対しては過小評価した。本実験により、数10MeV領域の系統的な実験データ整備が完了したため、今後は断面積の入射エネルギー依存性等を解析し、計算コードの高度化に貢献する。


Simulation study on the design of nondestructive measurement system using fast neutron direct interrogation method to nuclear materials in fuel debris

前田 亮; 古高 和禎; 呉田 昌俊; 大図 章; 米田 政夫; 藤 暢輔

Journal of Nuclear Science and Technology, 56(7), p.617 - 628, 2019/07

 被引用回数:1 パーセンタイル:58.8(Nuclear Science & Technology)

In order to measure the amount of nuclear materials in the fuel debris produced in the Fukushima Daiichi Nuclear Power Plant accident, we have designed a measurement system based on a Fast Neutron Direct Interrogation (FNDI) method. In particular, we have developed a fast response detector bank for fast neutron measurements by Monte Carlo simulations. The new bank has more than an order of magnitude faster response compared to the standard ones. We have also simulated the nondestructive measurements of the nuclear materials in homogeneously mixed fuel debris with various matrices which contain Stainless Steel (JIS SUS304), concrete, and various control-rod (CR) contents in the designed system. The results show that at least some types of the fissile materials in the debris can be measured by using the designed system.


Development of active neutron NDA system for radioactive nuclear materials

藤 暢輔; 大図 章; 土屋 晴文; 古高 和禎; 北谷 文人; 米田 政夫; 前田 亮; 小泉 光生

Proceedings of INMM 60th Annual Meeting (Internet), 7 Pages, 2019/07

Nuclear material accountancy plays a key role in nuclear safeguards and security. The collaboration between the Japan Atomic Energy Agency (JAEA) and the Joint Research Centre (JRC) of the European Commission aims to develop an active neutron NDA system for Special Nuclear Materials (SNM) and Minor Actinides (MA) in highly radioactive nuclear materials. Several active neutron NDA techniques, namely Differential Die-Away Analysis (DDA), Prompt Gamma-ray Analysis (PGA), Neutron Resonance Capture Analysis (NRCA), Neutron Resonance Transmission Analysis (NRTA) and Delayed Gamma-ray Analysis (DGA) have been developed. The different methods can provide complementary information. In the first phase of the project, we developed a combined NDA system, which enables the simultaneous measurements of DDA and PGA. The DDA technique can determine very small amounts of the fissile mass. PGA is valuable for the measurement of light elements. In the second phase, we will continue to conduct additional research to improve the methodology and develop a new integrated NDA system which can use for NRTA as well as DDA and PGA. In this presentation, we will provide an overview of the project and report the recent results, especially the design of new integrated NDA system. This research was implemented under the subsidiary for nuclear security promotion of MEXT.


Measurement of neutron-production double-differential cross sections of $$^{rm nat}$$C, $$^{27}$$Al, $$^{rm nat}$$Fe, and $$^{rm nat}$$Pb by 20, 34, 48, 63, and 78 MeV protons in the most-forward direction

佐藤 大樹; 岩元 洋介; 小川 達彦

Nuclear Instruments and Methods in Physics Research A, 920, p.22 - 36, 2019/03

 被引用回数:1 パーセンタイル:58.8(Instruments & Instrumentation)

原子力機構が中心となり開発を進める粒子輸送計算コードPHITSは、加速器施設の遮蔽設計をはじめとして、多くの分野で利用されている。しかし、PHITSで用いられる核反応模型や核データは、陽子入射反応における最前方方向の中性子生成を適切に再現できないことが知られていた。そこで、本研究では、PHITSによる計算モデルの高精度化に資するため、20から78MeVの 陽子入射による$$^{rm nat}$$C, $$^{27}$$Al, $$^{rm nat}$$Feおよび$$^{rm nat}$$Pbの最前方方向における中性子生成二重微分断面積の実験データを取得した。量子科学技術研究開発機構のイオン照射研究施設(TIARA)において、サイクロトンから供給される陽子と標的物質との核反応で生成した中性子のうち、最前方方向に開くコリメータを通したフラックスと運動エネルギーを測定した。実験結果をPHITSの計算結果と比較したところ、計算で用いるINCLおよびJENDL-4.0/HEは原子核の離散的なエネルギー準位間の遷移を考慮していないため、軽核で観測されたピーク構造を再現できないことが分かった。また、エネルギー積分断面積に対して、JENDL-4.0/HEは実験値とファクター2以内で一致するが、INCLは最大で6倍程度大きな値を与えることが分かった。


Establishment of a novel detection system for measuring primary knock-on atoms

Tsai, P.-E.; 岩元 洋介; 萩原 雅之*; 佐藤 達彦; 小川 達彦; 佐藤 大樹; 安部 晋一郎; 伊藤 正俊*; 渡部 浩司*

Proceedings of 2017 IEEE Nuclear Science Symposium and Medical Imaging Conference (NSS/MIC 2017) (Internet), 3 Pages, 2018/11

一次はじき出し原子(PKA)のエネルギースペクトルは、モンテカロル放射線輸送コードを用いた加速器施設設計の放射線損傷評価において重要である。しかし、計算コードに組み込まれている物理モデルは、PKAスペクトル について実験値の不足から十分に検証されていない。これまで、従来の固体検出器を用いた原子核物理実験の測定体系において、劣った質量分解能や核子あたり数MeV以上と高い測定下限エネルギーのため、実験値は限られていた。そこで本研究では、粒子・重イオン輸送計算コードPHITSを用いて、PKAスペクトルを測定するための2つの時間検出器と1つのdE-Eガス検出器からなる新しい測定体系を設計した。その結果、本測定体系は、質量数20から30のPKAにおいて、核子当たり0.3MeV以上のエネルギーを持つPKA同位体を区別できる。一方で、質量数20以下のPKAにおいては、PKAの質量数を識別できる下限エネルギーは核子当たり0.1MeV以下に減少する。今後、原子力機構のタンデム施設、及び東北大学のサイクロトロン・ラジオアイソトープセンターにおいて、設計した測定体系の動作テストを行う予定である。


Development of differential die-away technique in an integrated active neutron NDA system for nuclear non-proliferation and nuclear security

大図 章; 前田 亮; 米田 政夫; 藤 暢輔; 小泉 光生; 瀬谷 道夫

Proceedings of 2017 IEEE Nuclear Science Symposium and Medical Imaging Conference (NSS/MIC 2017) (Internet), 4 Pages, 2018/11

A Differential Die-away Analysis (DDA) system using a compact pulsed neutron (14 MeV) generator has been newly developed for non-nuclear proliferation and nuclear security in the Japan Atomic Energy Agency (JAEA). The DDA system was designed to be able to detect a nuclear fissile material (Pu-239) of as low as 10 mg and to handle samples of a different volume: a vial bottle (20 mL), a pail container (20 L), through a Monte Carlo simulation. In the DDA system, the Fast Neutron Direct Interrogation (FNDI) technique, which utilizes fast neutrons for interrogation, was applied to measure the amount of fissile mass contained in the sample. The fundamental performance of the DDA system was investigated in the demonstration experiment. The simulation results show that the Pu-239 masses of less than 10 mg can be detected in the DDA system. The results of the experiment are discussed and compared with those of the simulation.


Measurement of displacement cross sections of aluminum and copper at 5 K by using 200 MeV protons

岩元 洋介; 吉田 誠*; 義家 敏正*; 佐藤 大樹; 八島 浩*; 松田 洋樹; 明午 伸一郎; 嶋 達志*

Journal of Nuclear Materials, 508, p.195 - 202, 2018/09

 被引用回数:5 パーセンタイル:21.94(Materials Science, Multidisciplinary)



Experimental validation of the brightness distribution on the surfaces of coupled and decoupled moderators composed of 99.8% parahydrogen at the J-PARC pulsed spallation neutron source

原田 正英; 勅使河原 誠; 大井 元貴; Klinkby, E.*; Zanini, L.*; Batkov, K.*; 及川 健一; 藤 暢輔; 木村 敦; 池田 裕二郎

Nuclear Instruments and Methods in Physics Research A, 903, p.38 - 45, 2018/09

 被引用回数:4 パーセンタイル:29.78(Instruments & Instrumentation)

At the J-PARC pulsed spallation neutron source, liquid hydrogen moderators composed of 99.8% parahydrogen associated with light-water premoderator have been providing high intensity cold and thermal neutron beams. In the design stage, simulations have shown not only high total neutron intensity in the coupled moderator but also a local neutron-brightness increase at the edges. The edge-effect-brightness increase is also exploited in the design of the European Spallation Source (ESS) moderators, which are based on 99.8% parahydrogen, but thin (thickness: 3 cm) to enhance the neutron brightness. In this study, the spatial distribution of the neutron brightness at the surface of the coupled moderator in the J-PARC pulsed spallation neutron source was directly measured with the pinhole geometry to validate the calculated edge-brightness enhancement. The brightness distribution at the moderator surface was clearly observed as predicted by a Monte Carlo simulation, proving the validity of the simulation tools used in the design-optimization process of the J-PARC and ESS moderator.


Corrigendum; Study of the neutron multiplication effect in an active neutron method [J Nucl Sci Technol. 2017;54(11):1233-1239]

米田 政夫; 大図 章; 森 貴正; 中塚 嘉明; 前田 亮; 呉田 昌俊; 藤 暢輔

Journal of Nuclear Science and Technology, 55(8), P. 962, 2018/08

 被引用回数:0 パーセンタイル:100(Nuclear Science & Technology)

以前に発表した論文(アクティブ中性子法における中性子増倍効果に関する研究(J Nucl Sci Technol. 2017;54(11):1233-1239)における式の導出法を訂正する。式の導出法に間違いがあったが、最終的に導出される式は正しい。そのため、論文の結論及び議論に変更は無い。


Study on neutron beam pulse width dependence in the nuclear fuel measurement by the neutron resonance transmission analysis

北谷 文人; 土屋 晴文; 藤 暢輔; 堀 順一*; 佐野 忠史*; 高橋 佳之*; 中島 健*

KURRI Progress Report 2017, P. 99, 2018/08

As a non-destructive analytical technique for nuclear material in the field of nuclear security and nuclear nonproliferation, a neutron resonance transmission analysis (NRTA) attracts attention of researchers. It is important to downsize a NRTA system when it is deployed at various facilities. For this aim, we have developed a compact NRTA system which utilizes a D-T neutron generator. Its pulse width of 10$$mu$$s is much longer than that of a large electron beam accelerator. It is necessary to understand the influence of pulse widths on the NRTA measurement. Therefore, we conducted the experiments of the simulated nuclear fuel pin samples to evaluate how the NRTA measurement is influenced by the pulse width of neutron beam. Experiments were performed in Kyoto University. The simulated fuel pellet sample was made from metallic powders of Ag (around 1%) and Al (around 99%). The energy of the irradiation neutron is determined by a Time of Flight technique. We used three pulse widths of the neutron beam of 0.1, 1 and 4 $$mu$$s. A resonance dip of $$^{108}$$Ag at 5.19 eV is observed in the all spectra. And the dip of the TOF spectrum shifts towards low energy, with pulse width changed to a longer one. In this work, we confirmed that neutron pulse width affected the NRTA measurement of the fuel pin sample. On the basis of this work, we will be able to quantify the effects of long-pulse width in a resonance analysis.


Radiation damage calculation in PHITS and benchmarking experiment for cryogenic-sample high-energy proton irradiation

岩元 洋介; 松田 洋樹; 明午 伸一郎; 佐藤 大樹; 中本 建志*; 吉田 誠*; 石 禎浩*; 栗山 靖敏*; 上杉 智教*; 八島 浩*; et al.

Proceedings of 61st ICFA Advanced Beam Dynamics Workshop on High-Intensity and High-Brightness Hadron Beams (HB 2018) (Internet), p.116 - 121, 2018/07



Neutron resonance transmission analysis for measurement of nuclear materials in nuclear fuel

土屋 晴文; 北谷 文人; 藤 暢輔; Paradela, C.*; Heyse, J.*; Kopecky, S.*; Schillebeeckx, P.*

Proceedings of INMM 59th Annual Meeting (Internet), 6 Pages, 2018/07

In fields of nuclear safeguards and nuclear security, non-destructive assay (NDA) techniques are needed in order to quantify special nuclear materials (SNMs) in nuclear fuels. Among those techniques, active NDA ones would be preferable to passive ones. One candidate of active NDA techniques is neutron resonance transmission analysis (NRTA). In fact, experiments done at GELINA have shown that NRTA has high potential enough to quantify SNMs in complex materials. Currently, such a NRTA system requires a large electron accelerator facility to generate intense neutron sources. In other words, it is very difficult to perform NRTA at various facilities that need to measure SNMs. Thus, downsizing a NRTA system would be one solution of its difficulty. In order to realize a compact NRTA system, we develop a prototype with a D-T neutron generator that has a pulse width of 10 $$mu$$s. For this aim, numerical calculations to optimize the compact NRTA system were done. In addition, NRTA measurements with simulated fuel pins were made at neutron time-of-flight facilities such as GELINA. In this presentation, we present results of the numerical calculations and the experimental results. On the basis of those results we discuss a future prospect of a compact NRTA system that would be applicable to SNM quantification. This research was implemented under the subsidiary for nuclear security promotion of MEXT.

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