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Microscopic dynamics of lithium diffusion in single crystal of the solid-state electrolyte La$$_{2/3-x}$$Li$$_{3x}$$TiO$$_{3}$$ (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 La$$_{2/3-x}$$Li$$_{3x}$$TiO$$_{3}$$ (LLTO) with $$x = 0.13$$. By using a large $$^{7}$$Li-enriched single crystal sample, a QENS signal was clearly observed along the three principal axes [110], [111], and [001] at a temperature ($$T$$) 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$$^{+}$$ ($$D_{rm Li}$$) 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 $$D_{rm Li}$$ with decreasing $$T$$ 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$$_{7}$$P$$_{3}$$S$$_{11}$$, with 10 times larger ionic conductivity, which clarifies how to understand the Li conduction mechanism in LLTO and Li$$_{7}$$P$$_{3}$$S$$_{11}$$ in a unified manner.


Charge-density-wave order and multiple magnetic transitions in divalent europium compound EuAl$$_4$$

金子 耕士; 川崎 卓郎; 仲村 愛*; 宗像 孝司*; 中尾 朗子*; 花島 隆泰*; 鬼柳 亮嗣; 大原 高志; 辺土 正人*; 仲間 隆男*; et al.

Journal of the Physical Society of Japan, 90(6), p.064704_1 - 064704_6, 2021/06

 被引用回数:2 パーセンタイル:72.06(Physics, Multidisciplinary)

Multiple transition phenomena in divalent Eu compound EuAl$$_4$$ with the tetragonal structure were investigated via single crystal time-of-flight neutron Laue technique. At 30 K below a charge-density-wave (CDW) transition, superlattice peaks emerge near nuclear Bragg peaks described by an ordering vector $$q_{rm CDW}$$ = (0 0 $${delta}_c$$). In contrast, magnetic peaks appear at $$q_2 = ({delta}_2 {delta}_2 0)$$ with $${delta}_2$$ = 0.09 below $$T_{N1}$$ = 15.4 K, and moves to $$q_1 = ({delta}_1 0 0)$$ with $${delta}_1$$ = 0.19 below $$T_{N3}$$ =12.2 K, whereas no distinct change in the magnetic Bragg peak was detected at $$T_{N2}$$ and $$T_{N4}$$. The structural modification with $$q_{rm CDW}$$ is characterized by an absence of the superlattice peak in (0 0 $$l$$). Considering an absence of splitting in magnetic peaks along $$l$$, the structural transition is mainly ascribed to a displacement of Al ions within the tetragonal $$ab$$-plane. Complex incommensurate magnetic transitions are in stark contrast to a simple collinear commensurate structure in isovalent EuGa$$_4$$. This could stem from incompatible electronic structures with the CDW transition between two compounds.


Correlated Li-ion migration in the superionic conductor Li$$_{10}$$GeP$$_{2}$$S$$_{12}$$

矢島 健*; 日沼 洋陽*; 堀 智*; 岩崎 類*; 菅野 了次*; 大原 高志; 中尾 朗子*; 宗像 孝司*; 広井 善二*

Journal of Materials Chemistry A, 9(18), p.11278 - 11284, 2021/05

 被引用回数:1 パーセンタイル:0(Chemistry, Physical)

Herein, we studied the crystalline compound Li$$_{10}$$GeP$$_{2}$$S$$_{12}$$ with the largest Li-ion conductivity thus far via a novel route based on a combination of single-crystal neutron diffraction experiments at low temperature and first-principles calculations, and found that a correlated migration of the densely packed Li ions governs the overall Li-ion conduction. The correlated migration mechanism provides us with guidelines on how to design efficient superionic conductors for more efficient batteries.


Mechanistic study on the removal of Cs from contaminated soil by rapid ion exchange in subcritical water

福田 達弥*; 高橋 亮*; 原 卓飛*; 尾原 幸治*; 加藤 和男*; 松村 大樹; 稲葉 優介*; 中瀬 正彦*; 竹下 健二*

Journal of Nuclear Science and Technology, 58(4), p.399 - 404, 2021/04

 被引用回数:1 パーセンタイル:0.01(Nuclear Science & Technology)

As a result of the Fukushima nuclear power plant accident in March 2011, massive amounts of soil were contaminated with radioactive Cs. To remediate the contaminated soil, we are developing a desorption technique for removing Cs from soil using subcritical water. We found that rapid ion exchange of Cs with multivalent cations in subcritical water is an effective desorption technique. To understand the mechanism and structural aspects of this process, in situ observations of the soil layer in subcritical water were carried out by high-energy X-ray diffraction together with pair distribution function analysis, and extended X-ray absorption fine structure analysis. Both the desorption experiments and structural studies indicated that conformational changes of the layer containing Cs$$^{+}$$ under subcritical water conditions promoted intercalation of the hydrated Mg and trapped Cs$$^{+}$$, which facilitated a rapid ion-exchange reaction of Mg$$^{2+}$$ and Cs$$^{+}$$.



与能本 泰介; 中島 宏*; 曽野 浩樹; 岸本 克己; 井澤 一彦; 木名瀬 政美; 長 明彦; 小川 和彦; 堀口 洋徳; 猪井 宏幸; et al.

JAEA-Review 2020-056, 51 Pages, 2021/03




断層変位地形が不明瞭なひずみ集中帯におけるリニアメントカタログの作成; 南九州せん断帯における事例(受託研究)

後藤 翠; 佐々木 亮道*; 小松 哲也; 三輪 敦志*; 照沢 秀司*; 楮原 京子*; 島田 耕史

JAEA-Research 2020-013, 88 Pages, 2020/11


活断層を見出す調査技術の向上は、地層処分事業を進めるにあたって、断層のずれに伴う透水性の増加が生じる場所を避ける観点から重要である。通常、活断層の存在は、断層運動の地形学的痕跡である断層変位地形の空中写真判読と、現地の地質調査により確認する。しかし、地形学的な痕跡が不明瞭な場合の調査手法は十分整備されていない。そこで、本研究では、既往の地形学的手法を高度化する観点から、活断層を見出す指標となり得る地形学的特徴の直線状ないし弧状配列(リニアメント)を、通常の活断層研究ではほとんど無視されるような明瞭さが乏しいランクまで判読した。調査地域は、測地学的なひずみ集中帯であり、1997年鹿児島県北西部地震(Mj 6.6)の震源断層が伏在している南九州せん断帯である。本研究では、1/25,000地形図62枚の範囲の空中写真判読を実施し、得られた1,327条のリニアメントを地形図上に示し、リニアメントの分布密度,方向性,長さ,地形,地質などの項目について整理した。その結果、南九州せん断帯方向の東西系のリニアメントが西部で卓越し、鹿児島県北西部地震の余震分布域ではリニアメントが高密度で分布することが明らかとなった。これらの結果とともに、明瞭さ,方向,長さなどと地形的特徴の組み合わせによる類型化に基づく代表的な13条のリニアメントについてカタログをとりまとめた。


Production of $$^{266}$$Bh in the $$^{248}$$Cm($$^{23}$$Na,5$$n$$)$$^{266}$$Bh reaction and its decay properties

羽場 宏光*; Fan, F.*; 加治 大哉*; 笠松 良崇*; 菊永 英寿*; 小森 有希子*; 近藤 成美*; 工藤 久昭*; 森本 幸司*; 森田 浩介*; et al.

Physical Review C, 102(2), p.024625_1 - 024625_12, 2020/08

 被引用回数:2 パーセンタイル:57.67(Physics, Nuclear)

The nuclide $$^{266}$$Bh was produced in the $$^{248}$$Cm($$^{23}$$Na,5n)$$^{266}$$Bh reaction at beam energies of 125.9, 130.6, and 135.3 MeV. Decay properties of $$^{266}$$Bh were investigated with a rotating wheel apparatus for $$alpha$$ and spontaneous fission (SF) spectrometry under low background conditions attained by a gas-jet transport system coupled to the RIKEN gas-filled recoil ion separator. The half-life of $$^{266}$$Bh was measured to be $$T_{rm 1/2}$$ = 10.0$$^{+2.6}_{-1.7}$$ s. The $$alpha$$-particle energies of $$^{266}$$Bh disperse widely in the range of 8.62 - 9.40 MeV. The maximum production cross section for the $$^{248}$$Cm($$^{23}$$Na,5n)$$^{266}$$Bh reaction was determined to be $$sigma$$ = 57 $$pm$$ 14 pb at 130.6 MeV.


Successive phase transitions in $$R_{3}$$Ir$$_{4}$$Sn$$_{13}$$ ($$R$$: La and Ce) investigated using neutron and X-ray diffraction

中里 晟也*; 岩佐 和晃*; 橋本 大輔*; 塩澤 真未*; 桑原 慶太郎*; 中尾 裕則*; 佐賀山 基*; 石角 元志*; 大原 高志; 中尾 朗子*; et al.

JPS Conference Proceedings (Internet), 30, p.011128_1 - 011128_6, 2020/03

Successive phase transitions of $$R_{3}$$Ir$$_{4}$$Sn$$_{13}$$ ($$R$$: La and Ce) were studied using neutron and X-ray diffraction techniques. A semimetal Ce$$_{3}$$Ir$$_{4}$$Sn$$_{13}$$ undergoes three phase transitions: an antiferromagnetic ordering characterized by a propagation vector $$q_{rm M}$$ = (1/2, 1/2, 2/5) below 0.6 K, a structural transformation with $$q_{rm S2}$$= (1/4, 1/4, 1/4) at 2.0 K, and another structural transformation with $$q_{rm S1}$$ = (1/2, 1/2, 0) above room temperature. La$$_{3}$$Ir$$_{4}$$Sn$$_{13}$$ was confirmed to be a superconductor below 2.5 K under the $$q_{rm S1}$$ = (1/2, 1/2, 0) structure that also appears above room temperature.


Crystal structure and cation distribution of the X-type hexaferrite Sr$$_{2}$$Co$$_{2}$$Fe$$_{28}$$O$$_{46}$$

駒淵 舞*; 漆原 大典*; 浅香 透*; 福田 功一郎*; 大原 高志; 宗像 孝司*; 石川 喜久*

Journal of the Physical Society of Japan, 89(3), p.034601_1 - 034601_5, 2020/03

 被引用回数:0 パーセンタイル:0(Physics, Multidisciplinary)

The crystal structure of an X-type hexaferrite Sr$$_{2}$$Co$$_{2}$$Fe$$_{28}$$O$$_{46}$$ was investigated by the X-ray and neutron diffraction methods for a single crystal. Sr$$_{2}$$Co$$_{2}$$Fe$$_{28}$$O$$_{46}$$ has the crystal structure described as a space group $$Roverline{3}m$$ ($$Z = 3$$) and its lattice constants are $$a$$ = 5.9165(2) ${AA}$; and $$c$$ = 84.1395(33) ${AA}$; at 843 K. Co ions are almost localized in the octahedral site ($$9d$$) in the middle of S$$^{*}$$S$$^{*}$$ blocks. In addition, the adjacent octahedral and tetrahedral sites to $$9d$$ site contain the significant number of Co$$^{2+}$$.


Heavy fermion state of YbNi$$_2$$Si$$_3$$ without local inversion symmetry

中村 翔太*; 兵頭 一志*; 松本 裕司*; 芳賀 芳範; 佐藤 仁*; 上田 茂典*; 三村 功次郎*; 斉木 克祥*; 磯 孝斉*; 山下 穣*; et al.

Journal of the Physical Society of Japan, 89(2), p.024705_1 - 024705_5, 2020/02

 被引用回数:1 パーセンタイル:32.18(Physics, Multidisciplinary)

We have succeeded in growing a new heavy fermion compound YbNi$$_2$$Si$$_3$$ by the flux method. From electrical resistivity, magnetization, specific heat, magnetic torque and X-ray photoemission measurements concluded that this compound is a heavy fermion compound exhibiting an antiferromagnetic order at 0.35 K.


Multi-step magnetic transitions in EuNiIn$$_4$$

池田 修悟*; 金子 耕士; 田中 佑季*; 川崎 卓郎; 花島 隆泰*; 宗像 孝司*; 中尾 朗子*; 鬼柳 亮嗣; 大原 高志; 望月 健生*; et al.

Journal of the Physical Society of Japan, 89(1), p.014707_1 - 014707_7, 2020/01

 被引用回数:0 パーセンタイル:0(Physics, Multidisciplinary)

Magnetism in EuNiIn$$_4$$ has been studied by specific heat, magnetic susceptibility, magnetization, $$^{151}$$Eu M$"o$ssbauer spectroscopy, and neutron diffraction experiments. The specific heat shows two magnetic transitions at $$T_{rm N1}$$ and $$T_{rm N2}$$ at zero magnetic field. An antiferromagnetic ground state of EuNiIn$$_4$$ has a uniaxial magnetic anisotropy along the b-axis, revealed by the magnetic susceptibility and the M$"o$ssbauer spectroscopy. Single crystal neutron diffraction experiments clarify that this antiferromagnetic structure in the ground state is characterized by the commensurate propagation vector $$q$$ = (1/2, 1/2, 1/2) which reveals no distinct anomaly at $$T_{rm N2}$$. The magnetization curve along the b-axis at 2 K shows four successive magnetic field-induced transitions up to 50 kOe and, reaches 7 $${mu}_{rm B}$$/f.u. above 190 kOe, The magnetic phase diagram in EuNiIn$$_4$$ has unique characteristics with five magnetic states in low magnetic field.


Short- and middle-ranges order structures of KNbO$$_3$$ nanocrystals

米田 安宏; 國定 諒一*; 近田 司*; 上野 慎太郎*; 藤井 一郎*; 永田 肇*; 尾原 幸治*; 和田 智志*

Japanese Journal of Applied Physics, 58(SL), p.SLLA03_1 - SLLA03_7, 2019/11

 被引用回数:2 パーセンタイル:22.92(Physics, Applied)

We studied KNbO$$_3$$ nanocrystals grown by a solvothermal method. Average and local structures were refined by combining Rietveld and PDF analysis. We found that a rhombohedrally distorted NbO$$_6$$ octahedron was maintained in short-range order region, even in the nanocrystals with a cubic average structure. The cubic structure of KNbO$$_3$$ nanocrystals were observed as a disordered phase of the rhombohedral structure. The disordered feature can be understood that the structural transformation owing to the particle-size effect is analogous to the temperature-driven phase transition.


Colossal barocaloric effects in plastic crystals

Li, B.*; 川北 至信; 河村 聖子; 菅原 武*; Wang, H.*; Wang, J.*; Chen, Y.*; 河口 沙織*; 河口 彰吾*; 尾原 幸治*; et al.

Nature, 567(7749), p.506 - 510, 2019/03

 被引用回数:85 パーセンタイル:99.22(Multidisciplinary Sciences)



Unique helical magnetic order and field-induced phase in trillium lattice antiferromagnet EuPtSi

金子 耕士; Frontzek, M. D.*; 松田 雅昌*; 中尾 朗子*; 宗像 孝司*; 大原 高志; 垣花 将司*; 芳賀 芳範; 辺土 正人*; 仲間 隆男*; et al.

Journal of the Physical Society of Japan, 88, p.013702_1 - 013702_5, 2019/01

 被引用回数:28 パーセンタイル:94.68(Physics, Multidisciplinary)

Magnetic transitions in chiral antiferromagnet EuPtSi were investigated by means of single crystal neutron diffraction. In the ground state, magnetic peaks emerge at positions represented by $$q_{1}$$=$$(0.2, 0.3, 0)$$. Upon heating, an additional magnetic peak splitting around 2.5 K was uncovered, indicating a presence of a first-order transition with $$q^*_{1}$$=$$(0.2, 0.3, {delta})$$. An half-polarized neutron scattering for polarization parallel to Q reveled that polarization antiparallel to Q has stronger intensity in both magnetic phases. This feature clarifies single chiral character of helical structure with moments normal to the ordering vector in both ordered states. Under vertical magnetic field along [1,1,1] in the $$A$$ phase, magnetic peaks form hexagonal patterns in the equatorial scattering plane around nuclear. An ordering vector $$q_{A}$$ of the $$A$$-phase has the similar size in the periodicity to $$q_{1}$$, and could be a hallmark of a formation of skyrmion lattice in EuPtSi.


Local structure and phase transitions of KNbO$$_3$$

米田 安宏; 尾原 幸治*; 永田 肇*

Japanese Journal of Applied Physics, 57(11S), p.11UB07_1 - 11UB07_6, 2018/11

 被引用回数:9 パーセンタイル:59.67(Physics, Applied)



Numerical simulation on self-leveling behavior of mixed particle beds using multi-fluid model coupled with DEM

Phan, L. H. S.*; 大原 陽平*; 河田 凌*; Liu, X.*; Liu, W.*; 守田 幸路*; Guo, L.*; 神山 健司; 田上 浩孝

Proceedings of 12th International Topical Meeting on Nuclear Reactor Thermal-Hydraulics, Operation and Safety (NUTHOS-12) (USB Flash Drive), 12 Pages, 2018/10



Structure analysis and derivation of deformed electron density distribution of polydiacetylene giant single crystal by the combination of X-ray and neutron diffraction data

田代 孝二*; 日下 勝弘*; 細谷 孝明*; 大原 高志; 塙坂 真*; 吉澤 功徳*; 山元 博子*; 新村 信雄*; 田中 伊知朗*; 栗原 和男*; et al.

Macromolecules, 51(11), p.3911 - 3922, 2018/06

 被引用回数:2 パーセンタイル:12.11(Polymer Science)

The crystal structure of polydiacetylene giant single crystal has been analyzed on the basis of the two different methods of wide-angle neutron diffraction and X-ray diffraction. The X-ray result gives us the total electron density distribution. The neutron result tells the positions of atomic nuclei. As a result, the so-called bonded (or deformed) electron density, i.e., the electron density distribution due to the conjugation among the covalently bonded atoms along the polymer chain, can be estimated using the two information. The present report is the first example of the application of X-N method to the synthetic polymer species.


Local structure analysis of KNbO$$_3$$ nanocrystals with cubic shape

米田 安宏; 國定 諒一*; 近田 司*; 上野 慎太郎*; 尾原 幸治*; 和田 智志*

Transactions of the Materials Research Society of Japan, 43(2), p.93 - 96, 2018/04



Liquid-like thermal conduction in intercalated layered crystalline solids

Li, B.; Wang, H.*; 川北 至信; Zhang, Q.*; Feygenson, M.*; Yu, H. L.*; Wu, D.*; 尾原 幸治*; 菊地 龍弥*; 柴田 薫; et al.

Nature Materials, 17(3), p.226 - 230, 2018/03

 被引用回数:71 パーセンタイル:96.98(Chemistry, Physical)

As a generic property, all substances transfer heat through microscopic collisions of constituent particles. A solid conducts heat through both transverse and longitudinal acoustic phonons, but a liquid employs only longitudinal vibrations. As a result, a solid is usually thermally more conductive than a liquid. In canonical viewpoints, such a difference also serves as the dynamic signature distinguishing a solid from a liquid. Here, we report liquid-like thermal conduction observed in the crystalline AgCrSe$$_{2}$$. The transverse acoustic phonons are completely suppressed by the ultrafast dynamic disorder while the longitudinal acoustic phonons are strongly scattered but survive, and are thus responsible for the intrinsically ultralow thermal conductivity. This scenario is applicable to a wide variety of layered compounds with heavy intercalants in the van der Waals gaps, manifesting a broad implication on suppressing thermal conduction. These microscopic insights might reshape the fundamental understanding on thermal transport properties of matter and open up a general opportunity to optimize performances of thermoelectrics.


Neutron scattering study of yttrium iron garnet

社本 真一; 伊藤 孝; 大西 弘明; 山内 宏樹; 稲村 泰弘; 松浦 直人*; 赤津 光洋*; 樹神 克明; 中尾 朗子*; 茂吉 武人*; et al.

Physical Review B, 97(5), p.054429_1 - 054429_9, 2018/02

 被引用回数:10 パーセンタイル:63.24(Materials Science, Multidisciplinary)


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