アルファ微粒子の実測に向けた単一微粒子質量分析法の高度化(委託研究); 令和3年度英知を結集した原子力科学技術・人材育成推進事業

廃炉環境国際共同研究センター; 大阪大学*

JAEA-Review 2023-039, 71 Pages, 2024/03

JAEA-Review-2023-039.pdf:4.43MB

日本原子力研究開発機構(JAEA)廃炉環境国際共同研究センター(CLADS)では、令和3年度英知を結集した原子力科学技術・人材育成推進事業(以下、「本事業」という)を実施している。本事業は、東京電力ホールディングス株式会社福島第一原子力発電所の廃炉等を始めとした原子力分野の課題解決に貢献するため、国内外の英知を結集し、様々な分野の知見や経験を、従前の機関や分野の壁を越えて緊密に融合・連携させた基礎的・基盤的研究及び人材育成を推進することを目的としている。平成30年度の新規採択課題から実施主体を文部科学省からJAEAに移行することで、JAEAとアカデミアとの連携を強化し、廃炉に資する中長期的な研究開発・人材育成をより安定的かつ継続的に実施する体制を構築した。本研究は、令和3年度に採択された研究課題のうち、「アルファ微粒子の実測に向けた単一微粒子質量分析法の高度化」の令和3年度分の研究成果について取りまとめたものである。本研究は、燃料デブリ取り出しの際に発生するウランやプルトニウムを含むアルファ微粒子のリアルタイムモニタリングに向け、単一微粒子質量分析法の高度化を目的とする。令和3年度において、質量分解能を向上する改良型単一微粒子質量分析計(ATOFMS)の開発に向けて、シミュレーションによりイオン軌道や飛行距離を最適化した結果、市販ATOFMSと比べて10倍以上の質量分解能ならびに9倍以上のイオン透過率が得られる構造を得、さらにそれに適合する粒子検出部の設計を完了した。また、検出効率を改善するために新たに開発する肥大化濃縮装置を設計し、それに必要な装置や部品を購入した。試作した肥大化部を用いて予備実験を行い、溶液から乾燥微粒子を製造できること等を確認した。模擬アルファ微粒子の粒径ならびに含有元素分布に関する研究。さらに、模擬アルファ微粒子の表面状態観測を実施し、気化・凝縮を経て生成したと考えられるサブmの粒径を持つ球状微粒子と、原料が飛散したと考えられる不定形の粒子が存在することを見出した。また、濃縮肥大化した粒子に対する表面状態等の性状分析も可能であることを見出した。

Laser-driven neutron generation realizing single-shot resonance spectroscopy

余語 覚文*; Lan, Z.*; 有川 安信*; 安部 勇輝*; Mirfayzi, S. R.*; Wei, T.*; 森 隆人*; Golovin, D.*; 早川 岳人*; 岩田 夏弥*; et al.

Physical Review X, 13(1), p.011011_1 - 011011_12, 2023/01

https://doi.org/10.1103/PhysRevX.13.011011

Neutrons are powerful tools for investigating the structure and properties of materials used in science and technology. Recently, laser-driven neutron sources (LDNS) have attracted the attention of different communities, from science to industry, in a variety of applications, including radiography, spectroscopy, security, and medicine. However, the laser-driven ion acceleration mechanism for neutron generation and for establishing the scaling law on the neutron yield is essential to improve the feasibility of LDNS. In this paper, we report the mechanism that accelerates ions with spectra suitable for neutron generation. We show that the neutron yield increases with the fourth power of the laser intensity, resulting in the neutron generation of in at a maximum, with Wcm, 900 J, 1.5 ps lasers. By installing a "hand-size" moderator, which is specially designed for the LDNS, it is demonstrated that the efficient generation of epithermal (0.1-100 eV) neutrons enables the single-shot analysis of composite materials by neutron resonance transmission analysis (NRTA). We achieve the energy resolution of 2.3% for 5.19-eV neutrons 1.8 m downstream of the LDNS. This leads to the analysis of elements and isotopes within sub-s times and allows for high-speed nondestructive inspection.

Effect of sample density in prompt -ray analysis

前田 亮; 瀬川 麻里子; 藤 暢輔; 遠藤 駿典; 中村 詔司; 木村 敦

Scientific Reports (Internet), 12(1), p.6287_1 - 6287_8, 2022/06

https://doi.org/10.1038/s41598-022-08594-2

A high-accuracy analytical method is broadly required to obtain reliable research results. Thus, prompt -ray analysis (PGA), one of the most accurate non-destructive analytical methods, has been employed in various fields. However, the measurement accuracy of PGA is also known to degrade in hydrogenous samples. The degradation is caused by variation in the measurement sensitivity (counts per milligram) following the change in neutron energy due to scattering with hydrogen nucleus. Number of scatterings is well known to depend on the hydrogen content in a sample. However, considering multiple scatterings, hydrogen density, which has not been taken into account as yet, may also lead to the accuracy degradation. In this research, the effect of the hydrogen density in PGA is investigated by evaluating the measurement sensitivity of samples with the same hydrogen content and different densities. The results showed that the measurement sensitivity varies by more than 30% depending on the hydrogen density even at the same hydrogen content. The variation is a particularly serious problem for PGA requiring a few percent accuracy in most cases. Additionally, although the variation is apparently observed in hydrogenous samples, the similar phenomenon can occur in other nuclides with a large scattering cross section; it may affect nuclear cross-section measurements using neutrons in such fields as astrophysics and nuclear energy.

KeV-region analysis of the neutron capture cross-section of Np

Rovira Leveroni, G.; 片渕 竜也*; 登坂 健一*; 松浦 翔太*; 児玉 有*; 中野 秀仁*; 岩本 修; 木村 敦; 中村 詔司; 岩本 信之

Journal of Nuclear Science and Technology, 59(1), p.110 - 122, 2022/01

https://doi.org/10.1080/00223131.2021.1954104

Neutron capture cross-section measurements for Np have been conducted with the Accurate Neutron Nucleus Reaction Measurement Instrument (ANNRI) at the Materials and Life Science Facility (MLF) of the Japan Proton Accelerator Research Complex (J-PARC) using neutrons with energy ranging from thermal energy to 1 MeV. A Time of Flight (TOF) method using a NaI(Tl) detector was employed for these measurements and the data were analyzed based on the pulse-height weighting technique in order to derive the neutron capture cross-section. The absolute capture cross-section was determined using the whole shape of the first resonance from JENDL-4.0 together with the total neutron flux derived from a Au sample measurement in which the first resonance was completely saturated. Both normalization techniques present agreement within 2%. The present results are also compared evaluated data libraries. There is a discrepancy of 10-25% discrepancy from 0.5 to 20 keV with JENDL-4.0. Nonetheless, above this energy, the JENDL-4.0 seems to reproduce the present data better as the results agree within uncertainties up to 500 keV. The cross-section results contain errors below 4% from 0.5 to 30 keV. However, the total uncertainty increases to over 8% over that energy. Along with the cross section measurement, theoretical calculations were performed to reproduce the present results.

Development of a neutron sintillator for a compact NRTA system

伊藤 史哲*; Lee, J.; 弘中 浩太; 高橋 時音; 鈴木 敏*; 堀 順一*; 寺田 和司*; 小泉 光生

KURNS Progress Report 2020, P. 98, 2021/08

文部科学省補助金事業「核セキュリティ強化等推進事業費補助金」の下、核不拡散技術開発の一環として、レーザー駆動中性子源(LDNS)を用いたコンパクトな核共鳴透過分析(NRTA)システムの技術開発を行っている。NRTAにおいては、パルス中性子源から放出される中性子エネルギーが、飛行時間(TOF)法を用いて測定される。LDNSは、短い飛行距離でも高精度なTOF測定を行うために必要となる、短いパルス幅を持つという特性等から注目されている。短距離TOF測定では、減速材中の水素への中性子捕獲による2.2MeVガンマ線の飛来タイミングと、共鳴エネルギー付近の中性子の飛来タイミングが重なり、大きなガンマ線背景事象が存在することとなる。また、LDNSは発展途上であるため、中性子フラックスが十分ではなく、検出効率の高い検出器を用いることが望ましい。このため、我々は、高エネルギーガンマ線に対する検出効率が低く、かつ高い中性子感度を持つ検出器(多層型中性子検出器)を開発してきた。令和3年度の実験結果の一つとして、多層型中性子検出器が、高エネルギーガンマ線に対して低感度であることが確かめられた。

Crystal chemistry of Sr-rich piemontite from manganese ore deposit of the Tone mine, Nishisonogi Peninsula, Nagasaki, southwest Japan

永嶌 真理子*; 佐野 優子*; 河内 貴子*; 赤坂 正秀*; 佐野 亜沙美

Journal of Mineralogical and Petrological Sciences, 115(5), p.391 - 406, 2020/10

https://doi.org/10.2465/jmps.191122

西彼杵半島利根鉱山の層状マンガン鉱床に産出するSrを含む紅簾石の結晶化学を調査した。電子顕微鏡、単結晶X線回折、Feメスバウアー分光、X線及び中性回折実験の手法を用いることで、Sr, Mn及びFeの各サイト占有率、およびSr含有量と紅簾石・緑簾石の構造変化の関係を明らかにした。

Measurement of Ge(n,) cross sections and implications for stellar nucleosynthesis

Lederer-Woods, C.*; Battino, U.*; Ferreira, P.*; Gawlik, A.*; 木村 敦; n_TOF Collaboration*; 他128名*

Physics Letters B, 790, p.458 - 465, 2019/03

https://doi.org/10.1016/j.physletb.2019.01.045

cross sections were measured at the neutron time-of-flight facility n_TOF at CERN up to neutron energies of 300 keV, providing for the first time experimental data above 8 keV. Results indicate that the stellar cross section at =30 keV is 1.5 to 1.7 times higher than most theoretical predictions. The new cross sections result in a substantial decrease of Ge produced in stars, which would explain the low isotopic abundance of Ge in the solar system.

Be(n,p)Li reaction and the cosmological lithium problem; Measurement of the cross section in a wide energy range at n_TOF at CERN

Damone, L.*; Barbagallo, M.*; Mastromarco, M.*; Cosentino, L.*; 原田 秀郎; 木村 敦; n_TOF Collaboration*; 他152名*

Physical Review Letters, 121(4), p.042701_1 - 042701_7, 2018/07

https://doi.org/10.1103/PhysRevLett.121.042701

We report on the measurement of the Be(n,p)Li cross section from thermal to approximately 325 keV neutron energy, performed in the high-flux experimental area (EAR2) of the n_TOF facility at CERN. This reaction plays a key role in the lithium yield of the big bang nucleosynthesis (BBN) for standard cosmology. The only two previous time-of-flight measurements performed on this reaction did not cover the energy window of interest for BBN, and they showed a large discrepancy between each other. The measurement was performed with a Si telescope and a high-purity sample produced by implantation of a Be ion beam at the ISOLDE facility at CERN. While a significantly higher cross section is found at low energy, relative to current evaluations, in the region of BBN interest, the present results are consistent with the values inferred from the time-reversal Li(p,n)Be reaction, thus yielding only a relatively minor improvement on the so-called cosmological lithium problem. The relevance of these results on the near threshold neutron production in the p+Li reaction is also discussed.

Measurement of the neutron capture cross-section of Cs as a part of the ImPACT project

Hales, B. P.; 中村 詔司; 木村 敦; 岩本 修

JAEA-Conf 2017-001, p.199 - 203, 2018/01

https://doi.org/10.11484/jaea-conf-2017-001

As part of the ImPACT project, it is currently planned to measure the neutron cross-section of Cs (half-life y), a long-lived fission product (LLFP), via neutron time-of-flight (TOF) method at the Japan Proton Accelerator Research Complex (J-PARC). Both Cs (natural Cs, stable) and Cs (half-life y) are unavoidable contaminants in the Cs sample. In working towards the measurement of Cs, a measurement of non-radioactive Cs has been conducted. The neutron capture cross-section of Cs in the thermal to epithermal energy region was experimentally measured via neutron TOF method at J-PARC. Measured results show good agreement with JENDL in the energy region below 10 eV.

Measurement of the Pu(n,f) cross-section at the CERN n_TOF facility; First results from experimental area II (EAR-2)

Stamatopoulos, A.*; Tsinganis, A.*; Colonna, N.*; 原田 秀郎; 木村 敦; n_TOF Collaboration*; 他126名*

EPJ Web of Conferences, 146, p.04030_1 - 04030_4, 2017/09

https://doi.org/10.1051/epjconf/201714604030

The accurate knowledge of the neutron-induced fission cross-sections of actinides and other isotopes involved in the nuclear fuel cycle is essential for the design of advanced nuclear systems, such as Generation-IV nuclear reactors. Such experimental data can also provide the necessary feedback for the adjustment of nuclear model parameters used in the evaluation process, resulting in the further development of nuclear fission models. In the present work, the Pu(n,f) cross-section was measured at CERN n_TOF facility relative to the well-known U(n,f) cross section, over a wide range of neutron energies, from meV to almost MeV, using the time-of-flight technique and a set-up based on Micromegas detectors. This measurement was the first experiment to be performed at n_TOF new experimental area (EAR-2), which offers a significantly higher neutron flux compared to the already existing experimental area (EAR-1).Preliminary results as well as the experimental procedure, including a description of the facility and the data handling and analysis, are presented.