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廣田 夕貴*; 富永 大輝*; 川端 隆*; 川北 至信; 松尾 康光*
Bioengineering (Internet), 9(10), p.599_1 - 599_17, 2022/10
被引用回数：0 パーセンタイル：0.01(Biotechnology & Applied Microbiology)Chitosan, which is an environmentally friendly and highly bio-producible material, is a potential proton-conducting electrolyte for use in fuel cells. Thus, to microscopically elucidate proton transport in hydrated chitosan, we employed the quasi-elastic neutron scattering (QENS) technique. QENS analysis showed that the hydration water, which was mobile even at 238 K, moved significantly more slowly than the bulk water, in addition to exhibiting jump diffusion. Furthermore, upon increasing the temperature from 238 to 283 K, the diffusion constant of water changed increased from 
to 
cm
/s. It was also found that a portion of the hydrogen atoms in chitosan undergo a jump-diffusion motion similar to that of the hydrogen present in water. Moreover, QENS analysis revealed that the activation energy for the jump-diffusion of hydrogen in chitosan and in the hydration water was 0.30 eV, which is close to the value of 0.38 eV obtained from the temperature-dependent proton conductivity results. Overall, it was deduced that a portion of the hydrogen atoms in chitosan dissociate and protonate the interacting hydration water, resulting in the chitosan exhibiting proton conductivity.
大政 義典*; 高木 茂幸*; 戸嶋 健人*; 横山 凱乙*; 遠藤 亘*; 折茂 慎一*; 齋藤 寛之*; 山田 武*; 川北 至信; 池田 一貴*; et al.
Physical Review Research (Internet), 4(3), p.033215_1 - 033215_9, 2022/09
Quasielastic neutron scattering (QENS) and neutron powder diffraction of the complex transition metalhydrides Li
MoH
and Li
NbH were measured in a temperature range of 10-300 K to study their structures and dynamics, especially the dynamics of the hydrogen atoms. These hydrides contain unusual ninefold H coordinated complex ions (MoH
or NbH
) and hydride ions (H
). A QENS signal appeared 
150 K due to the relaxation of H atoms. The intermediate scattering functions derived from the QENS spectra are well fitted by a stretched exponential function called the Kohlrausch-Williams-Watts functions with a small stretching exponent 
0.3-0.4, suggesting a wide relaxation time distribution. The 
dependence of the elastic incoherent structure factor is reproduced by the rotational diffusion of MH
(M = Mo or Nb) anions. The results are well supported by a van Hove analysis for the motion of H atoms obtained using first-principles molecular dynamics calculations. We conclude that the wide relaxation time distribution of the MH rotation is due to the positional disorder of the surrounding Li ions and a unique rotation with MH anion deformation (pseudorotation).
GeP
S
by quasi-elastic neutron scattering measurements堀 智*; 菅野 了次*; Kwon, O.*; 加藤 祐樹*; 山田 武*; 松浦 直人*; 米村 雅雄*; 神山 崇*; 柴田 薫; 川北 至信
Journal of Physical Chemistry C, 126(22), p.9518 - 9527, 2022/06
被引用回数：2 パーセンタイル：75.4(Chemistry, Physical)Understanding Li-ion conduction in superionic conductors accelerates the development of new solid electrolytes to enhance the charge-discharge performances of all-solid-state batteries. We performed a quasi-elastic neutron scattering study on a model superionic conductor (Li
Ge
P
S, LGPS), to reveal its ion dynamics on an angstrom-scale spatial range and a pico-to-nanosecond temporal range. The observation of spectra at 298 K confirmed the high lithium diffusivity. The obtained diffusion coefficient was in the order of 10
cms
at temperatures 
338 K and was higher than the reported diffusion coefficient over a longer time scale, as determined by the pulse-field gradient nuclear magnetic resonance method. This difference indicates that there are impediments to ionic motion over a longer time scale. The dynamic behavior of the Li ions was compared with that observed for the Li
P
SO phase, which possesses the same crystal structure type, but a lower ionic conductivity. The LGPS phase possessed a high lithium mobility over a distance of 
10 
, as well as a larger fraction of mobile Li ions, thereby indicating that these features enhance lithium conduction over a longer spatial scale, which is important in all-solidstate batteries.
古池 美彦*; Ouyang, D.*; 富永 大輝*; 松尾 龍人*; 向山 厚*; 川北 至信; 藤原 悟*; 秋山 修志*
Communications Physics (Internet), 5(1), p.75_1 - 75_12, 2022/04
被引用回数：2 パーセンタイル：81.21(Physics, Multidisciplinary)Circadian clock proteins often reveal temperature-compensatory responses that counteract temperature influences to keep their enzymatic activities constant over a physiological range of temperature. This temperature-compensating ability at the reaction level is likely crucial for circadian clock systems, to which the clock proteins are incorporated, to achieve the system-level temperature compensation of the oscillation frequency. Nevertheless, temperature compensation is yet a puzzling phenomenon, since side chains that make up the clock proteins fluctuate more frequently due to greater thermal energy at higher temperature. Here, we investigated temperature influences on the dynamics of KaiC, a temperature-compensated enzyme (ATPase) that hydrolyzes ATP into ADP in the cyanobacterial circadian clock system, using quasielastic neutron scattering. The frequency of picosecond to subnanosecond incoherent local motions in KaiC was accelerated by a factor of only 1.2 by increasing the temperature by 10
C. This temperature insensitivity of the local motions was not necessarily unique to KaiC, but confirmed also for a series of temperature-sensitive mutants of KaiC and proteins other than clock-related proteins. Rather, the dynamics associated with the temperature-compensatory nature of the reaction- and system-level was found in global diffusional motions, which was suggested to regulate the temperature dependence of ATPase activity and dephosphorylation process presumably through changes in the hexamer conformation of KaiC. The spatiotemporal scale at which cross-scale causality of the temperature sensitivity is established is finite, and extends down to picosecond to subnanosecond dynamics only in a very limited part of KaiC, not in its entire part.
富永 大輝*; 佐原 雅恵*; 川北 至信; 中川 洋; 山田 武*
Journal of Applied Crystallography, 54(6), p.1631 - 1640, 2021/12
被引用回数：3 パーセンタイル：66.27(Chemistry, Multidisciplinary)For quasi-elastic neutron scattering (QENS) studies, sample cells made of pure or alloyed aluminum are frequently employed. Although the Al surface is protected by a passivating film, this film is not robust. Therefore, when the sample is an aqueous solution, chemical interactions between the Al surface and sample, promoted by corrosive entities such as chloride ions and certain conditions of pH, can compromise the integrity of the cell and interfere with the experiment. In this study, the corrosion susceptibilities of Al and its alloys were investigated by subjecting them to various treatments; the results were compared with those of other candidate materials with low chemical reactivity. This work showed that alloys with higher Al content and boehmite-coated surfaces are resistant to corrosion. In particular, for Al, the resistance is due to a reduction in the contact area achieved by reducing the surface roughness. QENS measurements of empty sample cells made of these materials revealed two results: (1) the profile of the cell fabricated with a copper-free Al alloy showed a minor dependence on the scattering vector magnitude and (2) reducing the real surface area of Al effectively suppresses its scattering intensity, while boehmite coating strengthens the scattering. Cells fabricated with Mo, Nb and single-crystal sapphire can be used as alternatives to Al because of their low scattering intensity and reduced dependence on .
中村 惇平*; 川北 至信; 下村 浩一郎*; 末益 崇*
Journal of Applied Physics, 130(19), p.195701_1 - 195701_7, 2021/11
被引用回数：1 パーセンタイル：17.6(Physics, Applied)Hydrogen defects sometimes form shallow impurity levels in semiconductors, and it is an important topic for semiconductor research to investigate their details. One of the experimental methods to determine the state of hydrogen is the muon spin rotation (
SR) experiment. By observing formation of a pseudo-hydrogen atom, called muonium, it is possible to investigate the hydrogen defect levels. In a previous theoretical study, the pinning levels were calculated for various materials as a reference for hydrogen defect levels, and these levels were universally distributed near the hydrogen electrode potential. Based on the prediction, SR experiments were performed for germanium sulfide (GeS) and germanium telluride (GeTe), where the hydrogen electrode potential is located in the bandgap for GeS, but not for GeTe. As a result, the SR spectra showed that the muonium forms in GeS, while it does not in GeTe. In GeS, 58
of the muons formed muoniums. The activation energy was obtained as 
meV. The hyperfine coupling frequency was 
GHz, and the Bohr radius of muonium was 1.3 times larger than that in vacuum. These properties indicated that the identified muonium does not form a typical impurity level that affects the electrical properties.
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
被引用回数：2 パーセンタイル：29.21(Chemistry, Physical)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 . 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.
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
被引用回数：2 パーセンタイル：34.91(Materials Science, Multidisciplinary)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.
中川 洋; 齋尾 智英*; 長尾 道弘*; 井上 倫太郎*; 杉山 正明*; 味戸 聡志; 富永 大輝*; 川北 至信
Biophysical Journal, 120(16), p.3341 - 3354, 2021/08
被引用回数：1 パーセンタイル：18.55(Biophysics)マルチドメインタンパク質は、溶液中で様々な構造を持つことができる。他の分子との相互作用により、そのうちの1つの構造が安定化し、ドメインダイナミクスが変化することが知られている。マルチドメインタンパク質の溶液中での構造を解明するためには、小角散乱法を用いることができる。中性子スピンエコー法は、ナノ秒・ナノメートルスケールでのドメインダイナミクスを解析するための有望な技術であるが、まだ開発途上である。本研究では、非干渉性散乱を用いて中性子スピンエコー法のデータから拡散運動や流体力学的相互作用の寄与を定量的に除去し、マルチドメインタンパク質MurDの3つの機能状態のドメインダイナミクスの違いを明らかにした。3つの状態間の違いは、2つのドメインモードによって説明できた。
川北 至信; 菊地 龍弥*; 田原 周太*; 中村 充孝; 稲村 泰弘; 丸山 健二*; 山内 康弘*; 河村 聖子; 中島 健次
JPS Conference Proceedings (Internet), 33, p.011071_1 - 011071_6, 2021/03
ヨウ化銅は高温固相で、ヨウ素イオンが作る面心立方格子の隙間を銅イオンが動く超イオン伝導体になることで知られている。溶融相でも、集団的あるいは協調的なイオンの運動を示す特徴がある。MDシミュレーションにおいて、銅イオンの拡散がヨウ素イオンより非常に速いこと分かっている。Cu-Cu部分構造因子にはFSDPと呼ばれる構造を持ち、銅の分布に中距離秩序があることを示している。さらに、Cu-Cu部分二体分布関数は、Cu-Iで形成される最近接分布に深く入り込んでいる。そうした溶融CuIの異常的振る舞いの原因を解明するために、J-PARCの物質・生命科学実験施設に設置されたディスクチョッパー分光器AMATERASを用いて、中性子準弾性散乱(QENS)実験を行った。構造可干渉性のQENSから得られた動的構造因子を理解するため、モード分布解析を行った。その結果、ヨウ素イオンの運動が局所的に閉じ込められた空間で揺らぐような運動であること、一方銅イオンはヨウ素イオンより速く拡散する運動をしていることが分かった。
富永 大輝*; 佐原 雅恵*; 川北 至信; 中川 洋; 島本 直伸*
JPS Conference Proceedings (Internet), 33, p.011094_1 - 011094_5, 2021/03
中性子準弾性散乱研究では、しばしばアルミもしくはアルミ合金製の試料容器が使われる。入射中性子の強度増大に伴って、研究領域は拡がり続けており、希薄な試料環境でもデータ取得は以前より速くなっている。そうした研究分野の一つに水を含むシステムが挙げられる。この研究では、アルミに関する温度効果を調べ、低温環境下でもアルミの腐食が起きることが分かった。その理由は、母材としてのアルミニウムと不動態フィルムとしての酸化アルミニウムの膨張係数の差による。
松浦 直人*; 山田 武*; 富永 大輝*; 小林 誠*; 中川 洋; 川北 至信
JPS Conference Proceedings (Internet), 33, p.011068_1 - 011068_6, 2021/03
飛行時間分析型後方散乱分光器DNAにおける散乱強度の位置依存性を調査した。垂直方向(位置敏感一次元検出器(PSD)のピクセル方向)と水平方向(PSD毎)の両方で周期的な構造が見られた。DNAに設置されたソラースリットとアナライザー結晶の設計値を超えた過度な湾曲が、強度分布の起源であると考えられる。我々は、強度の位置依存性と弾性散乱のエネルギーオフセットを系統的に補正できるソフトウェアを開発した。このソフトウェアにより、本来の散乱強度からのずれが補正でき、エネルギー分解能などのデータの質も向上させることができる。
富永 大輝*; 小林 誠*; 山田 武*; 松浦 直人*; 川北 至信; 笠井 聡*
JPS Conference Proceedings (Internet), 33, p.011095_1 - 011095_5, 2021/03
トップローディング型冷凍機用の垂直移動型試料交換機が、J-PARC MLFのBL02に設置された中性子分光器の利用支援のために開発された。PEACEと名付けられたこの試料交換機は、中性子照射位置での試料位置の再現性を、PEEKと呼ぶ物質でできたガイドを利用して制御している。3つの試料位置でのバックグラウンド散乱のプロファイルの変化は
1.6%以内であることが分かった。この結果は、垂直軸からの試料位置の偏差が0.3mmであることを考えると妥当である。
富永 大輝*; 川北 至信; 中川 洋; 山田 武*; 柴田 薫
JPS Conference Proceedings (Internet), 33, p.011086_1 - 011086_5, 2021/03
後方散乱型中性子分光器、特にJ-PARC MLFのBL02(DNA)分光器用に最適化された二重円筒型石英試料セルを開発した。一端を閉じられた石英ガラス管を0.55mmの厚みまで削り、内筒を底部の突起によって外筒に同芯になるように挿入する。この石英セルは、標準的に用いられているアルミセルの表面に触れさせたくない試料に用いられる。石英セルと標準アルミセルの容器散乱の効果を重水バッファ試料を使って中性子準弾性散乱実験(QENS)により確かめた。Qが1[1/A]未満の領域では石英セルとアルミ容器の弾性散乱プロファイルはほぼ同一であった。一方Qが1[1/A]以上の領域では、石英ガラスのFSDPのために、プロファイルが異なることが分かった。この領域では、吸収補正や石英セルの個々の厚みの差を考慮した解析が必要である。
glasses細川 伸也*; 川北 至信; Stellhorn, J. R.*; Pusztai, L.*; Blanc, N.*; Boudet, N.*; 池田 一貴*; 大友 季哉*
JPS Conference Proceedings (Internet), 33, p.011070_1 - 011070_7, 2021/03
銀イオン伝導体Ag
(GeSe)
のx=0.15, 0.28, 0.33, 0.50の試料について局所・中距離原子秩序がAXS, XRD, ND, RMCモデリングを組合せて調べられた。AXSとXRDで得られた結果にNDを加えることによって、もっともらしい部分構造と部分pdfを得ることができた。AXSとRMCによる以前の結果とは対照的に、多くのAg-Ge, Ge-Ge相関が第一近接殻内に見られるようになり、第一原理MDシミュレーションと一致する結果となった。GeとSeの配位数は、Agを考慮に入れなければ、すべてのAg濃度で8-
規則にほぼ乗っている。Ag濃度が増加すると、Ag周りのGeとSeの部分配位数が著しく増加し、一方Ag-Ag配位数はわずかに増加するのみである。このことは、Agの伝導経路がAg-Ag相関の第2近接を経由して形成されていることを示している。
Zhai, Y.*; Luo, P.*; 長尾 道弘*; 中島 健次; 菊地 龍弥*; 川北 至信; Kienzle, P. A.*; Z, Y.*; Faraone, A.*
Physical Chemistry Chemical Physics, 23(12), p.7220 - 7232, 2021/03
被引用回数：2 パーセンタイル：34.19(Chemistry, Physical)2-Propanol was investigated, in both the liquid and supercooled states, as a model system to study how hydrogen bonds affect the structural relaxation and the dynamics of mesoscale structures, of approximately several Angstroms, employing static and quasi-elastic neutron scattering and molecular dynamics simulation. Dynamic neutron scattering measurements were performed over an exchanged wave-vector range encompassing the pre-peak, indicative of the presence of H-bonding associates, and the main peak. The dynamics observed at the pre-peak is associated with the formation and disaggregation of the H-bonded associates and is measured to be at least one order of magnitude slower than the dynamics at the main peak, which is identified as the structural relaxation. The measurements indicate that the macroscopic shear viscosity has a similar temperature dependence as the dynamics of the H-bonded associates, which highlights the important role played by these structures, together with the structural relaxation, in defining the macroscopic rheological properties of the system. Importantly, the characteristic relaxation time at the pre-peak follows an Arrhenius temperature dependence whereas at the main peak it exhibits a non-Arrhenius behavior on approaching the supercooled state. The origin of this differing behavior is attributed to an increased structuring of the hydrophobic domains of 2-propanol accommodating a more and more encompassing H-bond network, and a consequent set in of dynamic cooperativity.
細川 伸也*; 川北 至信; Pusztai, L.*; 池田 一貴*; 大友 季哉*
Journal of the Physical Society of Japan, 90(2), p.024601_1 - 024601_12, 2021/02
被引用回数：0 パーセンタイル：0(Physics, Multidisciplinary)In order to improve the reliability of short- and intermediate-range atomic structures of Ge
Se glasses, high quality neutron diffraction data, in both the real and reciprocal spaces, were added to the existing anomalous X-ray scattering and X-ray diffraction datasets [Hosokawa et al., Phys. Rev. B 84, 014201 (2011)] for reverse Monte Carlo modeling. This addition proved to be highly effective for obtaining well-refined structural data and for revealing a close relationship between the compositional stiffness transition occurring at about 
= 0.20-0.26 and the partial structures. Although the 
and 
functions gradually change with varying , important indications on the stiffness transition are confirmed on the basis of the intermediate-range element-selective atomic structures (
) more clearly than it was possible by previous results. An abrupt decrease in terms of the the prepeak intensity of 
, a rapid disappearance of the Ge-Ge homopolar bonds, anomalies in the ratio of edge- and corner-sharing Ge(Se
)
tetrahedra, and characteristic changes in the tetrahedral connections with decreasing X across the so-called intermediate phase have all been observed.
C; Inelastic neutron scattering study玉造 博夢; 村上 洋一*; 倉本 義夫*; 佐賀山 基*; 松浦 直人*; 川北 至信; 松石 聡*; 鷲尾 康仁*; 井下 猛*; 浜田 典昭*; et al.
Physical Review B, 102(22), p.224406_1 - 224406_5, 2020/12
被引用回数：7 パーセンタイル：51.79(Materials Science, Multidisciplinary)Magnetic excitations in layered electride YC have been found by inelastic neutron scattering. We have observed weak but clear magnetic scattering around the wave number 
, but no magnetic order down to the lowest temperature measured (7 K). The imaginary part of the dynamical susceptibility deduced is well described by the Lorentz function of energy 
for each momentum . The width 
of the Lorentzian is proportional to 
with 
at 
K. We have also found that with increasing the magnetic form factor decays faster than that of a 
electron in a single Y atom, which indicates a more extended magnetic moment in YC. These results provide experimental evidence that the itinerant magnetism in YC originates from the anionic electrons that reside in the interlayers. The Curie-Weiss-like behavior of the magnetic susceptibility reported in YC is ascribed to the mode coupling effects of spin fluctuations.
井上 倫太郎*; 小田 隆*; 中川 洋; 富永 大輝*; 齋尾 智英*; 川北 至信; 清水 将裕*; 奥田 綾*; 守島 健*; 佐藤 信浩*; et al.
Scientific Reports (Internet), 10, p.21678_1 - 21678_10, 2020/12
被引用回数：3 パーセンタイル：21.65(Multidisciplinary Sciences)非干渉性中性子準弾性散乱(iQENS)は、タンパク質の内部ダイナミクスを調べるための魅力的な手法である。しかし、中性子ビームのフラックスが低いことや、iQENSプロファイルから内部ダイナミクスを抽出するための解析手法がないことが、生理的条件下(溶液中)での研究の障害となっていた。近年の中性子分光器の開発により、iQENSプロファイルから内部ダイナミクス,並進拡散,回転拡散を切り離すことが可能となった。本研究では、球状性蛋白質(GDP)と天然変性蛋白質(IDP)の溶液中での内部ダイナミクスを調べた。その結果、IDPの平均緩和時間はGDPよりも大きいことが分かった。IDPの内部ダイナミクスを詳細に解析した結果、IDPのmobileなH原子の割合はGDPよりもはるかに高いことが明らかになった。興味深いことに、mobileな水素原子の割合は、溶媒に曝された表面の水素原子の割合と密接に関連していることがわかった。iQENS研究では、タンパク質の分子構造に応じて、溶媒にさらされたアミノ酸残基が内部ダイナミクスを支配していることが示された。
analysis transformed from the inelastic neutron scattering data中村 充孝; 菊地 龍弥*; 川北 至信
Physica B; Condensed Matter, 567, p.61 - 64, 2019/08
被引用回数：0 パーセンタイル：0(Physics, Condensed Matter)最近、非弾性中性子散乱実験(INS)データから変換した実空間動的構造因子を用いた多結晶NaIのフォノンダイナミクスに関する研究報告を行った。この研究は、通常のINS実験条件(Q
5
)であっても、物理的に十分意味のある実空間ダイナミクス情報が得られることを示したものであり、これまでに蓄積されてきた大量のINSデータの再利用と新たな視点での研究推進を促すものである。今回の発表では、解析の適用可能性とその限界について詳しく議論する。
