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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：7 パーセンタイル：56.17(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
cm
s
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.
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
被引用回数：3 パーセンタイル：20.58(Chemistry, Physical)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。
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：4 パーセンタイル：28.78(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.
菊地 龍弥*; 川北 至信
Physica B; Condensed Matter, 567, p.51 - 54, 2019/08
被引用回数：0 パーセンタイル：0.00(Physics, Condensed Matter)Real time and real space analysis for quasielastic neutron scattering (QENS) by means of the regularization method to estimate a spectrum has been developed. In our formalism, a mediation function between a dynamic structure factor, 
, and a time-space correlation function, 
,is estimated to minimize the sum of the least square fitting term for in a 
space and the regularization term for in a 
space. On the application to liquid bismuth which shows complicate static local structure, it is shown that a distribution function for Gaussian superposition to represent has good characters as a mediating function. The calculated from the estimated mediation function showed a good agreement with the experimental 
even for small acoustic phonon excitation in a low region and gave more or less reasonable estimation of dynamic structure beyond the measured range. In addition of the main property of that the ability to focus onto the relaxation process at a specific atomic distance helped us to understand a complicated layered structure in liquid bismuth, possibility of easy separation of self-diffusion from coherent QENS is shown.
吉田 亨次*; 井上 拓也*; 鳥越 基克*; 山田 武*; 柴田 薫; 山口 敏男*
Journal of Chemical Physics, 149(12), p.124502_1 - 124502_10, 2018/09
被引用回数：4 パーセンタイル：16.28(Chemistry, Physical)異なる幾つかの、グリシン濃度, pH、および充填率(=グリシン溶液の質量/MCM-41の乾燥質量))をパラメーターとして、メソポーラスシリカ(MCM-41)に閉じ込められたグリシン水溶液の示差走査熱量測定、X線回折および準弾性中性子散乱(QENS)を305-180Kの温度範囲で実施して、グリシン水溶液の熱的挙動, 構造、および動的特性に対する閉じ込め効果を検討した。
NHPbILi, B.; 川北 至信; Liu, Y.*; Wang, M.*; 松浦 直人*; 柴田 薫; 河村 聖子; 山田 武*; Lin, S.*; 中島 健次; et al.
Nature Communications (Internet), 8, p.16086_1 - 16086_9, 2017/06
被引用回数：80 パーセンタイル：90.61(Multidisciplinary Sciences)Perovskite CHNHPbI exhibits outstanding photovoltaic performances, but the understanding of the atomic motions remains inadequate even though they take a fundamental role in transport properties. Here, we present a complete atomic dynamic picture consisting of molecular jumping rotational modes and phonons, which is established by carrying out high-resolution time-of-flight quasi-elastic and inelastic neutron scattering measurements in a wide energy window ranging from 0.0036 to 54 meV on a large single crystal sample, respectively. The ultrafast orientational disorder of molecular dipoles, activated at approximately 165 K, acts as an additional scattering source for optical phonons as well as for charge carriers. It is revealed that acoustic phonons dominate the thermal transport, rather than optical phonons due to sub-picosecond lifetimes. These microscopic insights provide a solid standing point, on which perovskite solar cells can be understood more accurately and their performances are perhaps further optimized.
