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Sm synchrotron-radiation-based M
ssbauer and 
SR studies of Sm
Ru
Ge
筒井 智嗣; 伊藤 孝; 中村 仁*; 吉田 実生*; 小林 義男*; 依田 芳卓*; 中村 惇平*; 幸田 章宏*; 東中 隆二*; 青木 大*; et al.
Interactions (Internet), 245(1), p.55_1 - 55_9, 2024/12
Sm SR-based Mssbauer and muon spin relaxation (SR) spectroscopies have been applied to SmRuGe. The temperature dependence of the Sm SR-based Mssbauer spectra in the paramagnetic state implies the presence of dynamical nuclear Zeeman and/or quadrupole interactions. The time differential SR spectra also exhibit a marked temperature dependence in the paramagnetic state, indicating the presence of magnetic fluctuation in SmRuGe at least. These results in the present work infer that the dynamical hyperfine interactions observed using the mutually complementary spectroscopic methods are connected with the mechanism of the heavy fermion behavior in SmRuGe.
Sm synchrotron-radiation-based Mssbauer spectroscopy of Sm-based heavy fermion compounds筒井 智嗣; 東中 隆二*; 水牧 仁一朗*; 小林 義男*; 中村 仁*; 伊藤 孝; 依田 芳卓*; 松田 達磨*; 青木 勇二*; 佐藤 英行*
Interactions (Internet), 245(1), p.9_1 - 9_10, 2024/12
Sm synchrotron-radiation-based Mssbauer spectroscopy has been applied to Sm-based heavy fermion intermetallics, Sm
Al
(
= Ti, V and Cr) and SmOs
Sb
. The isomer shifts obtained demonstrate that the Sm valence states in these compounds are intermediate. Since the difference of the isomer shifts in 22.502 keV Sm Mssbauer effect between Sm
and Sm
state is comparable to the 2nd order Doppler shift, consideration of the 2nd order Doppler shift is required to precisely discuss Sm valence state through the shifts of the Mssbauer spectra. In addition, the plots of the isomer shifts obtained by the Mssbauer spectroscopy against the Sm valence states estimated from Sm L-edge X-ray absorption spectroscopy exhibit a linear correlation except for that in SmOsSb. This implies that the origin of the intermediate valence state in SmOsSb differs from that in SmAl ( = Ti, V and Cr).
勅使河原 誠; Lee, Y.*; 達本 衡輝*; Hartl, M.*; 麻生 智一; Iverson, E. B.*; 有吉 玄; 池田 裕二郎*; 長谷川 巧*
Nuclear Instruments and Methods in Physics Research B, 557, p.165534_1 - 165534_10, 2024/12
被引用回数：0 パーセンタイル：0.00(Instruments & Instrumentation)J-PARCの核破砕中性子源において、水酸化第二鉄触媒の機能性を評価するため、1MW運転時の積算ビーム出力9.4MW
hの条件で、ラマン分光法を用いてパラ水素割合をその場測定した。その結果、1MW運転におけて触媒が十分に機能していることが分かった。また、触媒を通さないバイパスラインを用いて、中性子照射によるパラからオルソ水素への逆変換率を調べることを試みた。測定されたオルソ水素割合の増加は、500kW運転で積算ビーム出力2.4MWhの場合に0.44%であった。しかしながら、この結果は、冷中性子モデレータ内で引き起こされた逆変換と、バイパスされた触媒容器中の温度上昇によって発生した準静的オルソ水素のメインループへの受動的滲出との合算であることが示された。
Batsaikhan, M.; 大場 弘則; 狩野 貴宏; 赤岡 克昭; 若井田 育夫
Optics Express (Internet), 32(24), p.42626 - 42638, 2024/11
被引用回数：0A fiber-coupled, acoustic-wave-assisted microchip laser-induced breakdown spectroscopy system (AW-mLIBS) was developed to analyze the elemental composition and surface imaging. In this study, we measured the dependence of sample temperature and laser ablation angle on the laser-induced plasma-optical emission and LIP-acoustic signal. The intensity of the laser-induced plasma-optical emission and ablated mass at three different temperatures and eight different laser ablation angles were estimated using a zirconium sample. Simultaneously, we investigated the laser-induced plasma-acoustic signal amplitude, propagation speed, and shape by synchronizing the AW-mLIBS system with a high-speed camera. The results revealed that the laser-induced plasma-optical emission increases with increasing temperature and is unaffected by laser ablation angle up to 40 degree because the amount of the ablated mass was similar and the plasma. Additionally, no considerable variation in plasma temperature obtained using the Boltzmann method over the sample temperature. However, the propagation speed of the laser-induced plasma-acoustic signal differs with temperature but has marginal angular dependence because the laser-induced plasma-acoustic signal propagates as semispherical. Furthermore, small and no considerable changes observed in the laser-induced plasma-acoustic signal amplitude up to 100 degree Celsius, and the laser ablation angle showed a similar tendency to that of the laser-induced plasma-optical emission.
岩田 圭弘; 宮部 昌文; Wells, S. R.*; 山元 祐太*; 長谷川 秀一*
Proceedings of International Topical Workshop on Fukushima-Daiichi Decommissioning Research 2024 (FDR2024) (Internet), 4 Pages, 2024/10
本研究では、(i)レーザー偏光に依存した選択則及び(ii)奇数同位体の持つリュードベリレベルの大きな同位体シフトに着目して、奇数同位体分離を目指したCa原子の3段階及び2段階共鳴イオン化スキームを開発した。レーザー偏光が直交条件となる場合に、奇数同位体の分離を確認した。イオン化領域の電場による
Caの非共鳴イオン化を抑制することで、さらなる
Caの光学的同位体選択性向上が期待される。
田村 浩司; 中西 隆造; 大場 弘則; 狩野 貴宏; 柴田 卓弥; 平等 拓範*; 若井田 育夫
Journal of Nuclear Science and Technology, 61(8), p.1109 - 1116, 2024/08
被引用回数：1 パーセンタイル：30.19(Nuclear Science & Technology)For the development of the remote elemental analysis method in a radiation environment based on the laser-induced breakdown spectroscopy (LIBS), the radiation effects on the laser oscillation properties of the single crystal (SC) Nd: YAG microchip laser (MCL) were investigated and compared with those of ceramics Nd: YAG MCL. The laser oscillation properties were measured under gamma-ray irradiation as a function of dose rate. The effects on the SC MCL properties were found to be very small compared to those on the ceramics, indicating minimal radiation effects on the LIBS signal when using SC MCL. Pulse energy and oscillating build-up time (BUT) were measured for a cumulative dose exceeding 1400 kGy. The pulse energy remained stable, and the laser continued to oscillate under irradiation. The BUT also remained stable, demonstrating negligible optical loss accumulation that could affect laser properties even at the demonstrated cumulative dose. The results indicate that the effects of dose rate and cumulative dose on SC MCL laser properties were minimal. The SC MCL was then integrated into the LIBS system, and the gadolinium signal of composite oxides, simulating fuel debris, was successfully measured at the dose rate of 5 kGy/hr. These findings highlight the radiation tolerance of SC MCL as a laser medium for remote LIBS applications in harsh radiation environments.
Lan, Z.*; 有川 安信*; Mirfayzi, S. R.*; Morace, A.*; 早川 岳人*; 佐藤 博隆*; 加美山 隆*; Wei, T.*; 巽 湧太*; 小泉 光生; et al.
Nature Communications (Internet), 15, p.5365_1 - 5365_7, 2024/07
被引用回数：2 パーセンタイル：76.47(Multidisciplinary Sciences)The temperature measurement of material inside of an object is one of the key technologies for control of dynamical processes. For this purpose, various techniques such as laser-based thermography and phase-contrast imaging thermography have been studied. However, it is, in principle, impossible to measure the temperature of an element inside of an object using these techniques. One of the possible solutions is measurements of Doppler brooding effect in neutron resonance absorption (NRA). Here we present a method to measure the temperature of an element or an isotope inside of an object using NRA with a single neutron pulse of approximately 100 ns width provided from a high-power laser. We demonstrate temperature measurements of a tantalum (Ta) metallic foil heated from the room temperature up to 617 K. Although the neutron energy resolution is fluctuated from shot to shot, we obtain the temperature dependence of resonance Doppler broadening using a reference of a silver (Ag) foil kept to the room temperature. A free gas model well reproduces the results. This method enables element(isotope)-sensitive thermometry to detect the instantaneous temperature rise in dynamical processes.
Batsaikhan, M.; 赤岡 克昭; 佐伯 盛久*; 狩野 貴宏; 大場 弘則; 若井田 育夫
Journal of Nuclear Science and Technology, 61(5), p.658 - 670, 2024/05
被引用回数：2 パーセンタイル：51.90(Nuclear Science & Technology)この実験研究では、レーザー誘起ブレークダウン分光法(LIBS)を用いて模擬燃料デブリの二次元元素マッピングを実行し、サンプル表面の元素組成と分布を決定した。本物の燃料デブリはサンプルとして入手できないため、化合物や金属などの予測材料から模擬燃料デブリを作製した。Nd:YAGレーザーの第2高調波を使用して、サンプル表面にプラズマを生成させた。さらに、エシェル分光器を使用して、435
650nmの可視波長範囲でプラズマからの発光を検出した。収集されたデータセットのサイズと複雑さから従来のデータ分析方法では良い効果が得られないことが判明した。そのため本研究では、主成分分析や多変量曲線分解能代替最小二乗法などのラベルフリー化学測定法に基づく方法を実装して、サンプル内の各成分に関する空間情報およびスペクトル情報を取得した。結果として、LIBSと化学測定法の統合が、事前知識がほとんどまたは全く無くてもサンプル(燃料デブリなど)に関する定性情報を取得するための非常に効果的なツールであることを実証した。
線透過率差を利用した構造体内調査法の開発(委託研究); 令和4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; 京都大学*
JAEA-Review 2023-028, 54 Pages, 2024/03
JAEA-Review-2023-028.pdf:3.81MB
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4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(1F)の廃炉等をはじ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4年度に採択された研究課題のうち、「3次元線量拡散予測法の確立と線透過率差を利用した構造体内調査法の開発」の令和4年度分の研究成果について取りまとめたものである。我々は核ガンマ線の方向を完全に決定、光学カメラと同じ全単射によるガンマ線画像(線形画像)が測定できる電子飛跡検出型コンプトンカメラ(ETCC)を実現、今年、世界初の銀河拡散ガンマ線の直接観測に成功した。この特徴を生かし平成30年度英知事業に採択された「ガンマ線画像スペクトル分光法による高放射線場環境の画像化による定量的放射能分布解析法」(以下、前研究)では、1F免振棟から炉を含む1km四方を一度に撮像、約100か所のスペクトル測定を一度に実現、空からはスカイシャイン、炉からは662keVガンマ線が明瞭に測定でき、見晴台50
Sv/hでも無遮蔽で撮像に成功した。令和3年度には京都大学複合原子力科学研究所の原子炉建屋内の3次元線量測定を実施し、動作中の原子炉からのガンマ線の3次元撮像に成功した。さらに炉壁から放出された微量なArのガンマ線(1290keV)を動画で捉え、放射性物質拡散のガンマ線画像モニタリングが可能であることを実証した。本研究は、前研究の成果を基にサブmSv/h環境での3次元汚染物質飛散検知・予測システムの1F内で使用可能な実用化を行う。またETCCのMeV以上のガンマ線撮像能力を生かし透過性の高い
Csガンマ線を利用した炉建屋内の3次元透視Cs分布測定法を開発する。
-Ga
O
(001)Tsai, Y. H.*; 小畠 雅明; 福田 竜生; 谷田 肇; 小林 徹; 山下 良之*
Applied Physics Letters, 124(11), p.112105_1 - 112105_5, 2024/03
被引用回数：1 パーセンタイル：53.26(Physics, Applied)Recently, gallium oxide (GaO) has attracted much attention as an ultra-wide bandgap semiconductor with a bandgap of about 5 eV. In order to control device properties, it is important to clarify the chemical state of dopants and doping sites. X-ray absorption near edge structure (XANES) and hard X-ray photoemission spectroscopy were used to investigate the dopant sites and chemical states of Sn in Sn-doped -GaO(001) samples. The results show that the chemical state of the Sn dopant is the Sn
oxidation state and that the bond lengths around the Sn dopant atoms are longer due to the relaxation effect after Sn dopant insertion. Comparison of experimental and simulated XANES spectra indicates that the octahedral Ga substitution site in -GaO(001) is the active site of the Sn dopant.
Rodriguez, D.; Rossi, F.; 高橋 時音
IEEE Transactions on Nuclear Science, 71(3), p.255 - 268, 2024/03
被引用回数：0 パーセンタイル：0.00(Engineering, Electrical & Electronic)Under the MEXT subsidy to improve nuclear security related capabilities, we are developing the delayed gamma-ray spectroscopic analysis technique. One goal is to develop an inverse Monte Carlo analysis method using spectra from simulations of the interrogation instrument for comparison to the actual measured spectra. This work presents the validity of the Monte Carlo foundation of the analysis compared to experimental results and other simulation codes.
宮川 晃尚*; 林 直輝*; 岩本 響*; 新井 剛*; 長友 重紀*; 宮崎 康典; 長谷川 健太; 佐野 雄一; 中谷 清治*
Analytical Sciences, 40(2), p.347 - 352, 2024/02
被引用回数：1 パーセンタイル：14.27(Chemistry, Analytical)複数のランタノイドイオンを含む錯体溶液中における単一抽出剤含浸高分子被覆シリカ粒子中のEu(III)分配機構を蛍光顕微分光法を用いて調べた。律速段階はEu(III)と2つの抽出剤分子との反応であった。得られた機構と速度定数は、Eu(III)溶液中でEu(III)が粒子に分配される単元素系の機構と一致した。
岩田 圭弘; 宮部 昌文; 赤岡 克昭; 若井田 育夫; 長谷川 秀一*
Journal of the Optical Society of America B, 41(1), p.119 - 126, 2024/01
被引用回数：1 パーセンタイル：59.97(Optics)レーザー共鳴イオン化を用いてカルシウム41 (Ca)等の微量放射性核種を効率的かつ選択的に検出する上で、リュードベリ原子についての理解が必要不可欠である。本研究では、4sns 
S
及び4s(n-1)d D (n=40, 45, 50, 55, 60)リュードベリ準位について、イオン基底準位の超微細構造に起因したカルシウム43のエネルギーシフトを測定した。
鈴木 誠也; 勝部 大樹*; 矢野 雅大; 津田 泰孝; 寺澤 知潮; 小澤 孝拓*; 福谷 克之; Kim, Y.*; 朝岡 秀人; 柚原 淳司*; et al.
Small Methods, p.2400863_1 - 2400863_9, 2024/00
被引用回数：0 パーセンタイル：0.00(Chemistry, Physical)For group 14 monoelemental two-dimensional materials, such as silicene, germanene, and stanene, oxidation is a severe problem that alters or degrades their physical properties. This study shows that the oxidized germanene on Ag(111)/Ge(111) can be reformed to germanene by simple heating around 500 
C in a vacuum. The key reaction in reforming germanene is the desorption of GeO and GeO during heating around 350 C. After removing surface oxygen, Ge further segregates to the surface, resulting in germanene. The reformed germanene has the same crystal structure, a (7
7) R19.1 supercell with respect to Ag(111), and has equivalent high quality to that of as-grown germanene on Ag(111)/Ge(111). Even after air oxidation, germanene can be reformed by annealing in a vacuum. On the other hand, the desorption of GeO and GeO at high temperatures was not suppressed even in the O backfilling atmosphere. This instability of oxidized germanene/Ag(111)/Ge(111) at high temperatures contributes to the ease of germanene reformation without oxygen. In other words, the present germanene reformation, as well as the segregation of germanene on Ag(111)/Ge(111), is a highly robust process as a synthesis method of germanene.
McGrady, J.; 熊谷 友多; 渡邉 雅之; 桐島 陽*; 秋山 大輔*; 紀室 辰伍; 石寺 孝充
Journal of Nuclear Science and Technology, 60(12), p.1586 - 1594, 2023/12
被引用回数：2 パーセンタイル：51.90(Nuclear Science & Technology)Raman spectroscopy was used to investigate the effect of bicarbonate solution on the hyperstoichiometric UO surface oxide of UO pellets. The hyperstoichiometry causes distortion of the UO lattice, leading to the formation of defect peaks which arise in the Raman spectrum due to a loss of symmetry. By deconvolution of the defect peaks, the extent of oxygen inclusion and defect formation in the surface oxide as a function of bicarbonate concentration was investigated. Immersion in solution caused a reduction in the amount of interstitial oxygen due to dissolution U(V) and U(VI) in the UO oxide surface. The defect concentration increased upon immersion due to the formation of an equilibrium between dissolution and reprecipitation. The bicarbonate concentration affected the defect content which was attributed to different forms of U in solution (hydrolysed UO and UO(CO)
) leading to different rates of reduction and precipitation.
states in the electronic structure of the intermediate-valence superconductor CeIr藤森 伸一; 川崎 郁斗; 竹田 幸治; 山上 浩志; 雀部 矩正*; 佐藤 芳樹*; 清水 悠晴*; 仲村 愛*; Maruya, A.*; 本間 佳哉*; et al.
Electronic Structure (Internet), 5(4), p.045009_1 - 045009_7, 2023/11
The electronic structure of the 
-based superconductor 
was studied by photoelectron spectroscopy. The energy distribution of the 
state was revealed by the 
resonant photoelectron spectroscopy. The state was mostly distributed in the vicinity of the Fermi energy, suggesting the itinerant character of the state. The contribution of the state to the density of states (DOS) at the Fermi energy was estimated to be nearly half of that of the
states, implying that the state has aconsiderable contribution to the DOS at the Fermi energy. The 
core-level and X-ray absorption spectra were analyzed based on a single-impurity Anderson model. The number of the state in the ground state was estimated to be 0.8-0.9, which is much larger than the values obtained in the previous studies (i.e., 0-0.4).
Rodriguez, D.; Abbas, K.*; Bertolotti, D.*; Bonaldi, C.*; Fontana, C.*; 藤本 正己*; Geerts, W.*; 小泉 光生; Macias, M.*; Nonneman, S.*; et al.
Proceedings of INMM & ESARDA Joint Annual Meeting 2023 (Internet), 8 Pages, 2023/05
Under the MEXT subsidy to improve nuclear security related activities, we present the overview of the JAEA-JRC delayed gamma-ray spectroscopic analysis project. We describe past results, recent joint experiments, and the final goals for this project.
Rodriguez, D.; Rossi, F.
Proceedings of INMM & ESARDA Joint Annual Meeting 2023 (Internet), 9 Pages, 2023/05
Under the MEXT subsidy for the improvement of nuclear security related activities, we will present on the current and future progress of the delayed gamma-ray spectroscopic analysis development. We highlight a paper soon to be released and the plan for finalizing the project goal.
Rossi, F.; 小泉 光生; Rodriguez, D.; 高橋 時音
Proceedings of INMM & ESARDA Joint Annual Meeting 2023 (Internet), 5 Pages, 2023/05
Since 2015, the Integrated Support Center for Nuclear Nonproliferation and Nuclear Security (ISCN) of the Japan Atomic Energy Agency has been working on the development of the Delayed Gamma-ray Spectroscopy non-destructive assay technique for the quantification of fissile-nuclide content in mixed nuclear materials. Thanks to the efforts and lessons learned from past experiments, the ISCN has successfully designed and fabricated a final integrated instrument. The instrument is composed of a moderator and dose shield where different neutron sources, like Cf-252 and neutron generators, can be inserted to irradiate the sample. Within the moderator, a series of neutron detectors are installed for perform prompt neutron analysis and continuous monitoring of the neutron source emission. Thanks to an innovative transfer system, the sample is then moved to the gamma-ray detector in less than 1.5s providing a fast and reliable movement while being safe from possible contamination. In this work, we will describe the design details of this new instrument. This work is supported by the Japanese Ministry of Education, Culture, Sports, Science, and Technology (MEXT) under the subsidy for the "promotion for strengthening nuclear security and the like".
池田 裕二*; Soriano, J. K.*; 大場 弘則; 若井田 育夫
Scientific Reports (Internet), 13, p.4828_1 - 4828_9, 2023/03
被引用回数：12 パーセンタイル：95.62(Multidisciplinary Sciences)We report on the analysis of pure Gd oxide and its detection when mixed in surrogate nuclear debris using microwave-enhanced fiber-coupled micro-laser-induced breakdown spectroscopy. The target application is remote analysis of nuclear debris containing U inside the Fukushima Daiichi Nuclear Power Station. The surrogate nuclear debris used in this study contained Gd, Ce, Zr and Fe. The sample was ablated by microchip-laser under atmospheric pressure conditions while a helical antenna propagated 2.45 GHz 1.0 kW microwaves for 1.0 ms into the laser ablation plume. The results showed that microwave-induced plasma expansion led to enhanced emission signals of Gd I, Zr I, Fe I, Ce I, and Ce II. Microwave irradiation enhanced the standard deviations of the Gd and Ce emissions and lowered the detection limit of Gd by 60%.
