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Yang, J.*; Ren, W.*; Zhao, X.*; 菊地 龍弥*; Miao, P.*; 中島 健次; Li, B.*; Zhang, Z.*
Journal of Materials Science and Technology, 99, p.55 - 60, 2022/02
物性測定と中性子散乱を組み合わせることにより、面心立方高エントロピー合金CrMnFeCoNiの磁気および熱輸送特性を調べた。DCおよびAC帯磁率は、温度領域全体で反強磁性および強磁性相互作用が共存する常磁性挙動を示し、それぞれ、常磁性から反強磁性への遷移、反強磁性から強磁性への遷移、およびスピン凍結に対応して、約80, 50、および20Kで3つの異常が見られる。電気伝導率と熱伝導率はNiに比べて大幅に低下しており、格子熱伝導率の温度依存性はガラスのようなプラトーを示す。非弾性中性子散乱測定は弱い非調和性を示唆し、熱輸送は欠陥散乱によって支配されると思われる。
Naeem, M.*; He, H.*; Harjo, S.; 川崎 卓郎; Lin, W.*; Kai, J.-J.*; Wu, Z.*; Lan, S.*; Wang, X.-L.*
Acta Materialia, 221, p.117371_1 - 117371_18, 2021/12
We studied the deformation behavior of CrFeCoNi high-entropy alloy by in situ neutron diffraction at room temperature, intermediate low temperature of 140 K, low temperatures of 40 K (no serrated deformation) and 25 K (with massive serrations). The contributions from different deformation mechanisms to the yield strength and strain hardening have been estimated. The athermal contributions to the yield strength were 
183 MPa at all temperatures, while the Peierls stress increased significantly at low temperatures (from 148 MPa at room temperature to 493 MPa at 25 K). Dislocations contributed to 94% strain hardening at room temperature. Although the dislocation strengthening remained the major hardening mechanism at very low temperatures, the planar faults contribution increased steadily from 6% at room temperature to 28% at 25 K.
Klotz, S.*; Baptiste, B.*; 服部 高典; Feng, S. M.*; Jin, Ch.*; B
neut, K.*; Guigner, J. M.*; Est
ve, I.*
Carbon, 185, p.491 - 500, 2021/11
二硫化炭素(CS)は、その最も近い類似体であるCOとともに、二重共有結合からなる最も単純な分子系の一つである。高圧下では、この分子構造は分解され、拡張された結晶性またはポリマー性の固体を形成すると考えられる。ここでは、大容量高圧技術を用いて300Kで約10GPa (100kbar)まで圧縮することにより、瞬間的な反応で純粋な硫黄とCSに近い化学組成を持つ化合物の混合体が得られ、常圧まで回収できることを示している。中性子回折,X線回折,ラマン測定の結果、この物質は硫黄がナノメートルオーダーのsp
グラファイト層に結合していることがわかった。電気抵抗の温度依存性からこの化合物は45meVのギャップを持つ半導体であることが明らかになった。200
C以上の温度でアニールすることで、硫黄含有量をC
Sまで減らすことができた。この物質の構造的・電子的特性は、過去に行われたCSの高圧実験で報告された「ブリッジマンブラック」とは根本的に異なる。
橋本 俊輔*; 中島 健次; 菊地 龍弥*; 蒲沢 和也*; 柴田 薫; 山田 武*
Journal of Molecular Liquids, 342, p.117580_1 - 117580_8, 2021/11
エチレングリコール水溶液中に二酸化ケイ素(SiO
)ナノ粒子を分散したナノ流体の準弾性中性子散乱測定(QENS)およびパルス磁場勾配核磁気共鳴分析(PFGNMR)を行った。研究目的は、このナノ流体の熱伝導率が理論値を超えて増加するメカニズムを解明することだった。得られた実験結果は、SiOナノ粒子の周りの液体分子の運動が非常に制限されているため、SiOナノ粒子の添加により、エチレングリコール水溶液中の液体分子の自己拡散係数が低下していることを示す。そして温度一定の条件で、SiOナノ流体中で、液体分子の自己拡散係数が減少するにつれて、熱伝導率が増加した。
Kim, Y. S.*; Chae, H.*; Woo, W.*; Kim, D.-K.*; Lee, D.-H.*; Harjo, S.; 川崎 卓郎; Lee, S. Y.*
Materials Science & Engineering A, 828, p.142059_1 - 142059_10, 2021/11
CoCrNi medium entropy alloy (MEA) and stainless steel 316L (SS316L) were manufactured by direct energy deposition of additive manufacturing (DED-AM). Exceptional mechanical properties of DED CoCrNi at 210K were achieved by the activities of a multiple deformation scheme that changed from dislocation slip to twinning-induced plasticity followed by transformation-induced plasticity. While SS316L at room temperature has micro-twins, CoCrNi at 210K exhibited nano-twins, resulting from lower stacking fault energy. Moreover, transformed hexagonal close-packed (HCP) phases were found near the face-centered cubic (FCC) {111} grain boundaries, where remarkable stacking faults and severe lattice distortion were measured.
Tremsin, A. S.*; Gao, Y.*; Makinde, A.*; Bilheux, H. Z.*; Bilheux, J. C.*; An, K.*; 篠原 武尚; 及川 健一
Additive Manufacturing, 46, p.102130_1 - 102130_20, 2021/10
被引用回数：0Microstructures produced by Additive Manufacturing (AM) techniques determine many characteristics of components where these materials are used. Residual stress and texture are among those characteristics, which need to be optimized. In this study, we employ energy-resolved neutron imaging to investigate, non-destructively, the uniformity of texture and to map the distribution of strain due to residual stress in Inconel 625 samples. The samples used in this study were printed by a direct metal laser melting additive manufacturing technique. Strain and texture variation are measured at room temperature as well as their changes during annealing at 700C and 875C in a vacuum furnace. The uniformity of crystalline plane distribution, from which texture can be inferred, is imaged with sub-mm spatial resolution for the entire sample area.
伊藤 華苗; 山田 武*; 篠原 朗大*; 高田 慎一; 川北 至信
Journal of Physical Chemistry C, 125(39), p.21645 - 21652, 2021/10
The catalyst layer (CL) in polymer electrolyte fuel cells (PEFCs) plays a critical role in the performance of a PEFC. In this study, we investigate the water dynamics in the CL using quasielastic neutron scattering (QENS) and small-angle neutron scattering. The temperature dependence of the mean square displacement 
u
shows that the freezing of water does not occur at a melting temperature in the Nafion thin film of the CL, suggesting that the water is confined in a smaller region than 15 AA. The QENS measurements established three kinds of water in the CL: immobile water tightly connected to a sulfonic group, water in a fast mode assigned to free diffusion restricted in a sphere, and water in a slow mode described by a jump diffusion model. Assuming that these three modes were independent, the number of water molecules in each mode was estimated. On discussing the structure and dynamics elucidated in the study, we finally conclude that the coupled model of the fast and slow modes is plausible for describing the diffusion of water confined in the thin Nafion film of the CL.
Naeem, M.*; Zhou, H.*; He, H.*; Harjo, S.; 川崎 卓郎; Lan, S.*; Wu, Z.*; Zhu, Y.*; Wang, X.-L.*
Applied Physics Letters, 119(13), p.131901_1 - 131901_7, 2021/09
We investigated the in situ deformation behavior of the CrCoNi medium-entropy alloy at a cryogenic temperature of 140 K and compared it with deformation at room temperature. The sample exhibited higher strength and larger ductility at the cryogenic temperature. The CrCoNi alloy remained single-phase face-centered cubic at room temperature, while deformation at 140 K resulted in a martensitic transformation to the hexagonal close-packed structure. The phase transformation, an additional deformation mechanism to stacking faults, twinning, and dis- location slip, resulted in a higher work hardening at cryogenic temperature. The study addresses the structure metastability in the CrCoNi alloy, which led to the formation of epsilon-martensite from the intrinsic stacking faults.
Harjo, S.
検査技術, 26(9), p.9 - 13, 2021/09
変形下でのその場中性子回折実験が鋳鉄の変形挙動をどのように理解するために役立つかについて解説する。鋳鉄を繰り返し引張圧縮変形させるとなぜ強度が増すのかのメカニズムを調べるために、透過力の高い中性子を用いた回折実験を行い、試験片内部の原子配列を調べることで、それぞれの構成相に関連した回折線を定量的に解析し、各構成相が担う応力を求めた。繰り返し引張圧縮変形中に、「フェライト」において転位という結晶欠陥の蓄積が起こることで、「フェライト」の強度が高まった。そして、「フェライト」は、組織の割合がもっとも多いため、鋳鉄全体の強度を増大させた。「パーライト」の組織中に含まれている「セメンタイト」は、割合が2.2%しかないため、鋳鉄全体の強度への寄与は限られていた。一方、「球状黒鉛」は、驚くことに応力を負担せず、鋳鉄全体の強度へはほとんど寄与しない。
Tremsin, A. S.*; Bilheux, H. Z.*; Bilheux, J. C.*; 篠原 武尚; 及川 健一; Gao, Y.*
Nuclear Instruments and Methods in Physics Research A, 1009, p.165493_1 - 165493_12, 2021/09
被引用回数：1 パーセンタイル：0.03(Instruments & Instrumentation)The investigation of microstructure of crystalline materials is one of the possible and frequently used applications of energy-resolved neutron imaging. The position of Bragg edges is defined by sharp changes in neutron transmission and can thus be determined by the measurement of the transmission spectra as a function of neutron wavelength. The accuracy of this measurement depends on both the data analysis technique and the quality of the measured spectra. While the optimization of reconstruction methods was addressed in several previous studies, here we introduce an important prerequisite when aiming for high resolution Bragg edge strain imaging - a well calibrated flight path across the entire field of view (FOV). Compared to e.g. powder diffraction, imaging often uses slightly different geometries and hence requires a calibration for each particular setup. We herein show the importance of this calibration across the entire FOV in order to determine the instrumental error correction for pulsed neutron beamlines.
Gao, D.*; Tang, X.*; Wang, X.*; Yang, X.*; Zhang, P.*; Che, G.*; Han, J.*; 服部 高典; Wang, Y.*; Dong, X.*; et al.
Physical Chemistry Chemical Physics, 23(35), p.19503 - 19510, 2021/09
被引用回数：0窒素に富む分子の圧力有機相転移や重合は、環境にやさしい高エネルギー密度材料の開発にとって非常に重要であるため、広く注目されている。本論文では、その場ラマン,IR,X線回折,中性子回折、および理論計算をもちい、100GPaまでの1H-テトラゾールの相転移挙動と化学反応の研究を紹介する。2.6GPa以上での相転移が確認され、その高圧構造は、以前に報告されたユニットセル内に2つの分子をもつものではなく、1つの分子をものであることが分かった。1H-テトラゾールは、おそらく窒素-窒素結合ではなく炭素-窒素結合により、100GPa以下で可逆的に重合する。私たちの研究は、1H-テトラゾールの高圧相の構造モデルを更新し、もっともらしい分子間結合の経路を初めて提示した。これにより、窒素に富む化合物の相転移と化学反応の理解が進み、新しい高エネルギー密度材料の設計に役立つと考えられる。
Li
TiO
(x = 0.13) studied by quasielastic neutron scattering松浦 直人*; 藤原 靖幸*; 森分 博紀*; 尾原 幸治*; 川北 至信
Physical Review B, 104(9), p.094305_1 - 094305_7, 2021/09
Quasielastic neutron scattering (QENS) measurements combined with first principles based molecular dynamics calculations were conducted to study the dynamics of Li
ions in a solid-state electrolyte LaLiTiO (LLTO) with 
. By using a large 
Li-enriched single crystal sample, a QENS signal was clearly observed along the three principal axes [110], [111], and [001] at a temperature (
) of 600 K. Wave vector dependence of the linewidth of the QENS signal along each direction was explained well using the Chudley-Elliot model for jumps between the A sites of the perovskite lattice through the bottleneck square, which was also supported by molecular dynamics calculations. The estimated self-diffusion coefficient of Li (
) in the ab plane was slightly larger than that along the c axis, suggesting quasi-isotropic diffusion, that is, the three-dimensional diffusion of Li ions. The decrease in with decreasing was reasonably explained by a thermal activation process with the activation energy determined from ionic-conductivity measurements. Furthermore, the estimated values of the self-diffusion coefficient are comparable to those in the sulfide-based Li ion conductor, Li
PS
, with 10 times larger ionic conductivity, which clarifies how to understand the Li conduction mechanism in LLTO and LiPS in a unified manner.
足立 望*; 上野 春喜*; 尾上 勝彦*; 諸岡 聡; 戸高 義一*
ISIJ International, 61(8), p.2320 - 2322, 2021/08
被引用回数：0This study investigated the hydrogen permeation property of cementite by fabricating bulk cementite sample using the process combining the mechanical ball milling and subsequent pulse current sintering. The bulk cementite sample having a 96 vol% of cementite was successfully fabricated. The prepared bulk cementite showed no signal of hydrogen permeation during the 3.5 day of electrochemical hydrogen permeation test. The morphology of blister formed in the sample indicated that diffusion coefficient of hydrogen in cementite is very small.
丸山 龍治; 山崎 大; 青木 裕之; 阿久津 和宏*; 花島 隆泰*; 宮田 登*; 曽山 和彦; Bigault, T.*; Saerbeck, T.*; Courtois, P.*
Journal of Applied Physics, 130(8), p.083904_1 - 083904_10, 2021/08
被引用回数：0Ferromagnetic (FM) interlayer exchange coupling of ion-beam sputtered Fe/Ge multilayers was investigated by off-specular polarized neutron scattering measurements. We observed a monotonously growing correlation of magnetic moments in the out-of-plane direction with decreasing Ge thickness. The results of the Fe/Ge multilayers were used to invoke FM interlayer exchange coupling in a neutron polarizing supermirror in order to extend its bandwidth. Typically, the bandwidth is limited due to a Curie temperature close to room temperature of the thinnest Fe layers with less than 3 nm. We propose a modified layer sequence of the neutron polarizing supermirror, where the minimum Fe thickness was set to 3.5 nm whereas the Ge thickness was reduced. A performance test of the neutron polarizing supermirror showed that the FM interlayer exchange coupling contributed to the presence of the magnetization comparable to the bulk and resulted in a marked extension in the bandwidth.
南部 雄亮*; 社本 真一
Journal of the Physical Society of Japan, 90(8), p.081002_1 - 081002_15, 2021/08
被引用回数：0 パーセンタイル：0.01(Physics, Multidisciplinary)スピントロニクス用イットリウム鉄ガーネットの中性子散乱研究について、長期課題2017L0300の"Cross correlation dynamics under a strain field"の成果を中心にSPECIAL TOPICSのReviewとしてまとめた。
宮崎 司*; 宮田 登*; 有馬 寛*; 吉良 弘*; 大内 啓一*; 笠井 聡*; 津村 佳弘*; 青木 裕之
Langmuir, 37(32), p.9873 - 9882, 2021/08
被引用回数：0 パーセンタイル：0(Chemistry, Multidisciplinary)We investigated the structure of the crystalline adsorption layer of poly(vinyl alcohol) (PVA) in hot water by neutron reflectivity in two cases: when the adsorption layer is exposed on the substrate by leaching the upper bulk layer and when it is deeply embedded between a relatively thick PVA film and substrate. In both cases, the PVA adsorption layer consists of three layers on the Si substrate. The bottom layer, consisting of amorphous chains that are strongly constrained on the substrate, is not swollen even in hot water at 90C. The middle layer, consisting of amorphous chains that are much more mobile compared with those in the bottom layer, has no freedom to assume a crystalline form. Only the molecular chains in the top layer are crystallizable in the adsorption layer, leading to a heterogeneous layered structure in the film thickness direction. This layered structure is attributed to the crystallizable chains of PVA during the formation of the adsorption layer driven by hydrogen bonding. However, the structure and dynamics in the adsorption layer may differ in both cases because the molecular chains in the vicinity of the surface seem to be affected by surface effects even in the adsorption layer.
Vu, TheDang; 宍戸 寛明*; 相澤 一也; 小嶋 健児*; 小山 富男*; 及川 健一; 原田 正英; 奥 隆之; 曽山 和彦; 宮嶋 茂之*; et al.
Nuclear Instruments and Methods in Physics Research A, 1006, p.165411_1 - 165411_8, 2021/08
被引用回数：0 パーセンタイル：0.03(Instruments & Instrumentation)We found that the sizes of the Gd islands determined from the transmission image correlated strongly with those determined from the SEM image. We demonstrated the CB-KID could be used to identify (1) tiny voids in a thermally sprayed continuous GdO
film in and (2) various mosaic morphologies and different eutectic microstructures in Wood's metal samples. The fact that the CB-KID system could be used to identify features of samples with a wide distribution of sizes and thicknesses is promising for real application of the device for imaging samples of interest to material scientists. Operating the CB-KID at higher temperatures appreciably improved the efficiency for simultaneously identifying the X and Y positions of hotspots. We also compared the detection efficiency with the PHITS simulations. We now plan to improve the detection efficiency by increasing the thickness of the 
B neutron conversion layer
西村 昇一郎*; 鳥居 寛之*; 深尾 祥紀*; 伊藤 孝; 岩崎 雅彦*; 神田 聡太郎*; 川越 清以*; Kawall, D.*; 河村 成肇*; 黒澤 宣之*; et al.
Physical Review A, 104(2), p.L020801_1 - L020801_6, 2021/08
被引用回数：0As a method to determine the resonance frequency, Rabi-oscillation spectroscopy has been developed. In contrast to conventional spectroscopy which draws the resonance curve, Rabi-oscillation spectroscopy fits the time evolution of the Rabi oscillation. By selecting the optimized frequency, it is shown that the precision is twice as good as conventional spectroscopy with a frequency sweep. Furthermore, the data under different conditions can be treated in a unified manner, allowing more efficient measurements for systems consisting of a limited number of short-lived particles produced by accelerators such as muons. We have developed a fitting function that takes into account the spatial distribution of muonium and the spatial distribution of the microwave intensity to apply this method to ground-state muonium hyperfine structure measurements at zero field. It was applied to the actual measurement data, and the resonance frequencies were determined under various conditions. The result of our analysis gives 
= 4 463 301.61 
0.71 kHz.
Liss, K.-D.*; Harjo, S.; 川崎 卓郎; 相澤 一也; 徐 平光
Journal of Alloys and Compounds, 869, p.159232_1 - 159232_9, 2021/07
被引用回数：0 パーセンタイル：0.01(Chemistry, Physical)The aluminium strontium master alloy Al-10Sr has been investigated by in-situ neutron diffraction upon a heating-cooling cycle, revealing composition, crystallographic structure, lattice evolution and linear thermal expansion coefficients. Expansion of the Al matrix between (23.5 ... 26.7)
10
K
depends on temperature and fits well to the literature values, extrapolating to higher temperature at 800 K. Thermal expansion is highly anisotropic for tetragonal Al
Sr by a factor of 1.86 with values of 20.8 and 11.110 K in 
and 
-axis. The even large discrepancy to the Al matrix is prone to residual intergranular phase stresses, explaining the brittleness of such composite material. Upon first heating, recovery of the initially plastically deformed materials is observed until 600 K and 700 K, for AlSr and Al. Rietveld analysis refines the 4
Wyckoff positions of the 
4/
crystal structure to 
= 0.39 revealing that local tetrahedrons are regular while local hexagons are stretched, in contrast to the literature. Its lattice parameters report to 
= 4.44240(48) 
, 
= 11.0836(15) at 300 K. Furthermore, the manuscript demonstrates full technical analysis of the neutron data. Findings feed into data bases and an outlook for improving mechanical properties of AlSr composites is given.
川瀬 頌一郎*; 木村 敦; 原田 秀郎; 岩本 信之; 岩本 修; 中村 詔司; 瀬川 麻里子; 藤 暢輔
Journal of Nuclear Science and Technology, 58(7), p.764 - 786, 2021/07
被引用回数：0 パーセンタイル：0.02(Nuclear Science & Technology)The neutron capture cross sections of 
Cm and 
Cm were measured for the neutron energy range of 1-1000 eV via the neutron time-of-flight method with ANNRI at MLF of the J-PARC. The world's most intense neutron pulses from the Japan Spallation Neutron Source enable the accurate measurement of neutron capture cross sections. Besides, single-bunched neutron pulses allow the analysis in a higher neutron energy region than the previous measurement at ANNRI. The resonance analyses were performed up to 1000 eV by using a resonance shape analysis code REFIT. The spectra of prompt gamma-rays from neutron capture reactions of Cm and Cm were also obtained, and 43 and 10 prompt gamma-ray peaks from Cm(n,
) and Cm(n,) reactions were newly observed, respectively.
