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Local disorder in proton conductor BaSn$$_{0.5}$$In$$_{0.5}$$O$$_{2.75}$$ analyzed by neutron diffraction/ atomic pair distribution function

井川 直樹; 樹神 克明; 田口 富嗣*; 吉田 幸彦*; 松川 健*; 星川 晃範*; 石垣 徹*

Transactions of the Materials Research Society of Japan, 43(6), p.329 - 332, 2018/12

プロトン伝導体BaSn$$_{0.5}$$In$$_{0.5}$$O$$_{2.75}$$の電気的特性に及ぼす結晶構造の影響を理解するため、本材料における局所構造乱れを中性子回折/原子対分布関数(PDF)法を用いて解析した。本材料の局所構造は、${it r}$ $$>$$ 0.6nmの原子間距離範囲内では、リートベルト解析によって推定された平均構造と同様の立方晶構造(空間群$${it Pm}$$$$overline{3}$$$${it m}$$))である。一方、${it r}$ $$<$$ 0.6nmの範囲のPDFプロファイルは、立方晶構造よりも空間群${it P}$4/${it mmm}$の正方晶構造によって良い一致をみた。これらの結果は、格子内の局所構造乱れの存在を示している。本発表では、BaSn$$_{0.5}$$In$$_{0.5}$$O$$_{2.75}$$の平均構造と局所構造との関係の詳細について考察する。


High-energy spin fluctuation in low-T$$_{c}$$ iron-based superconductor LaFePO$$_{0.9}$$

石角 元志*; 社本 真一; 樹神 克明; 梶本 亮一; 中村 充孝; Hong, T.*; Mutka, H.*

Scientific Reports (Internet), 8, p.16343_1 - 16343_6, 2018/11

 パーセンタイル:100(Multidisciplinary Sciences)



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:1 パーセンタイル:100(Materials Science, Multidisciplinary)



Alternative equation on magnetic pair distribution function for quantitative analysis

樹神 克明; 池田 一貴*; 社本 真一; 大友 季哉*

Journal of the Physical Society of Japan, 86(12), p.124708_1 - 124708_8, 2017/12

 パーセンタイル:100(Physics, Multidisciplinary)

We derive an alternative equation of magnetic pair distribution function (mPDF) related to the mPDF equation given in a preceding study (B. A. Frandsen, X. Yang, and S. J. L. Billinge, Acta Crystallogr. A, ${bf70}$, 3 (2014)) for quantitative analysis of realistic experimental data. The additional term related to spontaneous magnetization included in the equation is particularly important for the mPDF analysis of ferromagnetic materials. Quantitative estimation of mPDF from neutron diffraction data is also shown. The experimental mPDFs estimated from the neutron diffraction data of the ferromagnet MnSb and the antiferromagnet MnF$$_2$$ are quantitatively consistent with the mPDFs calculated using the presented equation.


Local structural analysis of half-metallic ferromagnet CrO$$_2$$

樹神 克明; 池田 一貴*; 礒部 正彦*; 武田 晃*; 伊藤 正行*; 上田 寛*; 社本 真一; 大友 季哉*

Journal of the Physical Society of Japan, 85(9), p.094709_1 - 094709_5, 2016/09

 被引用回数:1 パーセンタイル:79.03(Physics, Multidisciplinary)

We have performed powder neutron diffraction on the half-metallic ferromagnet CrO$$_2$$ which has a rutile-type crystal structure with a tetragonal unit cell. Although the powder diffraction pattern can be fitted by the reported crystal structure including a single Cr site, the atomic pair distribution function (PDF) can be fitted by the structural model with an orthorhombic unit cell including two kinds of inequivalent Cr sites. The difference between the valences of the two inequivalent Cr sites, $$delta$$ of Cr$$^{+4pmdelta}$$, estimated from the local structural parameters is about 0.06. The shapes of the two CrO$$_6$$ octahedra are slightly different, suggesting the short-range orbital ordering of the Cr 3$$d$$ orbitals. The lattice distortion and the improvement of the fitting to the PDF obtained using the locally distorted structure model are apparent in the region below about 10 ${AA}$, suggesting that the domain size or correlation length of the locally distorted structure is about 10 ${AA}$, roughly corresponding to the size of two unit cells.


Observation of all-in type tetrahedral displacements in nonmagnetic pyrochlore niobates

鳥越 秀平*; 石本 祐太朗*; 青石 優平*; 村川 寛*; 松村 大樹; 吉井 賢資; 米田 安宏; 西畑 保雄; 樹神 克明; 富安 啓輔*; et al.

Physical Review B, 93(8), p.085109_1 - 085109_5, 2016/02

 被引用回数:3 パーセンタイル:66.42(Materials Science, Multidisciplinary)

We observed all-in type Nb tetrahedral displacement in nonmagnetic pyrochlore niobates A$$_{2}$$Nb$$_{2}$$O$$_{7}$$ (A = Nd$$_{0.5}$$Ca$$_{0.5}$$ and Y$$_{0.5}$$Ca$$_{0.5}$$) through the analysis of the neutron pair distribution function and the extended X-ray absorption function spectroscopy. The all-in type Nb tetrahedral displacement, which has the character of a charge singlet state, is driven by the formation of the bonding orbital. The diffuse scattering in the X-ray diffraction, which has the resonant component in the Nb $$L$$3 edge, indicates that the all-in type Nb tetrahedral displacement has the periodicity with its short-range correlation.


Synthesis of heterostructured SiC and C-SiC nanotubes by ion irradiation-induced changes in crystallinity

田口 富嗣; 山本 春也; 樹神 克明; 朝岡 秀人

Carbon, 95, p.279 - 285, 2015/12

 被引用回数:4 パーセンタイル:72.5(Chemistry, Physical)



Crystal structures and magnetic properties of nickel chain compounds PbM$$_2$$Ni$$_6$$Te$$_3$$O$$_{18}$$ (M = Mn, Cd)

土井 貴弘*; 鈴木 遼*; 日夏 幸雄*; 樹神 克明; 井川 直樹

Inorganic Chemistry, 54(22), p.10725 - 10731, 2015/11

 被引用回数:1 パーセンタイル:91.26(Chemistry, Inorganic & Nuclear)

The synthesis, crystal structures, and magnetic properties of the pentanary oxides PbM$$_2$$Ni$$_6$$Te$$_3$$O$$_{18}$$ (M = Mn and Cd) were investigated. These compounds crystallize in a hexagonal structure with space group $$P6_3/m$$, in which the Ni$$^{2+}$$ ions form a zigzag chain along the c axis. From the magnetic susceptibility and specific heat measurements, we found that the PbCd$$_2$$Ni$$_6$$Te$$_3$$O$$_{18}$$ behaves as a low-dimensional magnet due to the intrachain an tiferromagnetic interaction between Ni$$^{2+}$$ ions. Both compounds show a long-range antiferromagnetic ordering at 25.7 K (M = Cd) and 86.0 K (Mn). The magnetic structure of PbMn$$_2$$Ni$$_6$$Te$$_3$$O$$_{18}$$ determined by neutron diffraction measurements is a collinear antiferromagnetic arrangement of Mn$$^{2+}$$ ions in the Mn$$_2$$O$$_9$$ dimeric unit and Ni$$^{2+}$$ ions in the zigzag chain.


Local lattice distortion caused by short-range charge ordering in transition metal oxides

樹神 克明; 井川 直樹; 社本 真一; 池田 一貴*; 大下 英敏*; 金子 直勝*; 大友 季哉*; 鈴谷 賢太郎; 星川 晃範*; 石垣 徹*

JPS Conference Proceedings (Internet), 8, p.034002_1 - 034002_6, 2015/09

Cubic spinel compound LiMn$$_2$$O$$_4$$ with the mixed valence of Mn$$^{3.5+}$$ has non-metallic conductivity. The local structure determined by the PDF analysis has an orthorhombic lattice distortion and includes inequivalent Mn$$^{3+}$$ and Mn$$^{4+}$$ sites. YBaCo$$_2$$O$$_5$$ also exhibits non-metallic conductivity although the Co has the mixed valence of +2.5 above 220 K which corresponds with charge ordering temperature. The PDF obtained at 450 K is not reproduced by the PDF calculated for the averaged structure and can be reproduced by the PDF calculated for the structure model corresponding to the charge ordering state. These results suggest that the valence electrons are localized with short-range periodicity, resulting in the non-metallic conductivities in these materials.


Nuclear and electron density distributions of LiMn$$_{2}$$O$$_{4}$$ analyzed by combination of Rietveld/ maximum entropy method

井川 直樹; 樹神 克明; 美留町 厚; 田口 富嗣

e-Journal of Surface Science and Nanotechnology (Internet), 13, p.247 - 252, 2015/05

リチウムイオン電池用の正極材の一つであるLiMn$$_{2}$$O$$_{4}$$について、中性子回折およびX線回折法によるRietveld/最大エントロピー法解析を実施し、結晶構造とLiイオンの拡散経路を探査した。LiMn$$_{2}$$O$$_{4}$$の結晶構造は240$$sim$$573Kの温度域では${it Fd}$-3${it m}$であり、240K以下で${it Fddd}$へと相変化した。最大エントロピー法によって、LiMn$$_{2}$$O$$_{4}$$の原子核密度と電子密度分布を解析した結果、300KにおけるLiイオンは8${it b}$-16${it e}$サイト間を介して伝導していることが明らかになった。


Anisotropic magnetic form factor in a detwinned single crystal of BaFe$$_2$$As$$_2$$

樹神 克明; 石角 元志*; 脇本 秀一; 木方 邦宏*; Lee, C.-H.*; 伊豫 彰*; 永崎 洋*; 社本 真一

Physical Review B, 90(14), p.144510_1 - 144510_5, 2014/10

 被引用回数:1 パーセンタイル:92.3(Materials Science, Multidisciplinary)

We have performed neutron diffraction measurements at 12K on a single crystal of BaFe$$_2$$As$$_2$$, which serves as the parent compound of iron-based superconductor. To investigate the in-plane anisotropy of the magnetic form factor in the antiferromagnetic phase, the single crystal was detwinned. The magnetic structure factor and magnetic form factor are well explained by the spin densities comprising $$3d_{yz}$$ electrons with a fraction of approximately 40% and electrons in the other four $$3d$$ orbitals each with a fraction of approximately 15%. It is a direct observation of the largely anisotropic spin density relative to the small orthorhombic lattice distortion, $$(a-b)/(a+b)$$ $$sim$$ 0.3%.


Superconductivity in noncentrosymmetric iridium silicide Li$$_2$$IrSi$$_3$$

Pyon, S.*; 工藤 一貴*; 松村 純一*; 石井 博文*; 松尾 元太*; 野原 実*; 北條 元*; 岡 研吾*; 東 正樹*; Garlea, V. O.*; et al.

Journal of the Physical Society of Japan, 83(9), p.093706_1 - 093706_5, 2014/09

 被引用回数:13 パーセンタイル:26.29(Physics, Multidisciplinary)

The effects of lithium absorption on the crystal structure and electronic properties of IrSi$$_3$$, a binary silicide with a noncentrosymmetric crystal structure, were studied. X-ray and neutron diffraction experiments revealed that hexagonal IrSi$$_3$$ (space group $$P6_3mc$$) transforms into trigonal Li$$_2$$IrSi$$_3$$ (space group $$P31c$$) upon lithium absorption. The structure of Li$$_2$$IrSi$$_3$$ is found to consist of a planar kagome network of silicon atoms with Li and Ir spaced at unequal distances between the kagome layers, resulting in a polar structure along the c-axis. Li$$_2$$IrSi$$_3$$ exhibited type-II superconductivity with a transition temperature $$T_{rm c}$$ of 3.8 K, displaying a structure type that no previous superconductors have been reported to have.


Local structural analysis by using atomic pair distribution function on mixed valence compound LiMn$$_2$$O$$_4$$

樹神 克明; 井川 直樹; 社本 真一; 池田 一貴*; 大下 英敏*; 金子 直勝*; 大友 季哉*; 鈴谷 賢太郎; 星川 晃範*; 石垣 徹*

JPS Conference Proceedings (Internet), 3, p.013012_1 - 013012_6, 2014/06

LiMn$$_2$$O$$_4$$ has a cubic spinel structure with a single Mn site whose valence is +3.5. Below about 260 K, the compound exhibits a charge ordering and has inequivalent Mn sites with valences of +3 and +4. However, even in the cubic phase without the charge ordering, temperature dependence of the electrical conductivity is non-metallic. We have performed PDF (atomic pair distribution function) analysis on powder neutron diffraction data of LiMn$$_2$$O$$_4$$ obtained above 300 K where the compound has cubic structure. The local structure determined by PDF analysis has an orthorhombic lattice distortion and includes the inequivalent Mn sites with valences of +3 and +4 up to, at least, about 450 K. These results indicate that valence electrons are localized at Mn sites with short range periodicity, resulting in the non-metallic electrical conductivity. It can be regarded as a glass state of valence electrons whereas a charge ordering can be regarded as a crystallization of valence electrons.


2D neutron diffraction imaging on an ammonite

社本 真一; 樹神 克明; 伊巻 正*; 中谷 健; 大下 英敏*; 金子 直勝*; 増子 献児*; 坂本 健作; 山口 憲司; 鈴谷 賢太郎; et al.

JPS Conference Proceedings (Internet), 1, p.014011_1 - 014011_5, 2014/03



Magnetic structure and electromagnetic properties of LnCrAsO with a ZrCuSiAs-type structure (Ln = La, Ce, Pr, and Nd)

Park, S.-W.*; 溝口 拓*; 樹神 克明; 社本 真一; 大友 季哉*; 松石 聡*; 神谷 利夫*; 細野 秀雄*

Inorganic Chemistry, 52(23), p.13363 - 13368, 2013/12

 被引用回数:12 パーセンタイル:35.91(Chemistry, Inorganic & Nuclear)

We report the synthesis, structure, and electromagnetic properties of Cr-based layered oxyarsenides LnCrAsO (Ln = La, Ce, Pr, and Nd) with a ZrCuSiAs-type structure. All LnCrAsO samples showed metallic electronic conduction. Electron doping in LaCrAsO by Mnsubstitution for the Cr sites gave rise to a metal-insulator transition. Analysis of powder neutron diffraction data revealed that LaCrAsO had Gtype antiferromagnetic (AFM) ordering, i.e., a checkerboard-type AFM ordering in the CrAs plane and antiparallel spin coupling between the adjacent CrAs planes, at 300 K with a large spin moment of 1.57 $$mu_B$$ along the c axis. The magnetic susceptibility of LaCrAsO was very small (on the order of 10$$^{-3}$$ emu/mol) and showed a broad hump at $$sim$$550 K. First-principles density functional theory calculations of LaCrAsO explained its crystal structure and metallic nature well, but could not replicate the antiparallel spin coupling between the CrAs layers. The electronic structure of LaCrAsO is discussed with regard to those of related compounds LaFeAsO and LaMnAsO.


Local lattice distortion caused by short range charge ordering in LiMn$$_2$$O$$_4$$

樹神 克明; 井川 直樹; 社本 真一; 池田 一貴*; 大下 英敏*; 金子 直勝*; 大友 季哉*; 鈴谷 賢太郎

Journal of the Physical Society of Japan, 82(9), p.094601_1 - 094601_6, 2013/09

 被引用回数:6 パーセンタイル:46.59(Physics, Multidisciplinary)

We have performed powder neutron diffraction on $$^7$$LiMn$$_2$$O$$_4$$ at 300 K. The crystal structure determined by Rietveld analysis is a cubic spinel with space group of $$Fdbar{3}m$$ in which all Mn atoms are crystallograghically equivalent, consistent with many preceding studies. However, the atomic pair distribution function (PDF) of this compound cannot be fitted by the cubic structure satisfactorily, and it can be reproduced by the orthorhombic structure with $$Fddd$$. It corresponds with the structure of charge ordered phase below about 260 K, indicating a short range charge ordering. In the local structure determined by PDF analysis, two types of MnO$$_6$$ octahedra with long and short atomic distances between Mn and O atoms exist and their Mn-O distances are almost consistent with the distances in the charge ordered phase. From these results, valence electrons are localized at Mn sites like a glass even in the cubic phase, resulting in the non-metallic electrical conductivity.



大山 研司*; 樹神 克明; 井川 直樹

波紋, 23(2), p.147 - 153, 2013/05

This article gives an introduction of crystal and magnetic structure refinements using angular dispersive neutron powder diffractometers, HRPD and HERMES installed at JRR-3. Some useful information for material researchers who want to try neutron powder diffraction experiments is provided.


From antiferromagnetic insulator to ferromagnetic metal; Effect of hydrogen substitution in LaMnAsO

半那 拓*; 松石 聡*; 樹神 克明; 大友 季哉*; 社本 真一; 細野 秀雄*

Physical Review B, 87(2), p.020401_1 - 020401_5, 2013/01

 被引用回数:22 パーセンタイル:20.46(Materials Science, Multidisciplinary)

Manganese oxyarsenide hydrides LaMnAsO$$_{1-x}$$H$$_x$$ ($$x$$ = 0-0.73) were synthesized by a solid state reaction under a high pressure of 2 GPa. The hydride ions H$$^-$$ in O$$^{2-}$$ sites induced an insulator-to-metal conversion and suppressed the antiferromagnetic ordering of Mn spins. Instead, ferromagnetism with negative magnetoresistance was observed. The Curie temperature and saturated moment per Mn increased with $$x$$ up to 264 K and 1.5 $$mu_B$$, respectively, at $$x$$ = 0.73. These results indicate that H$$^-$$ donate conduction electrons to the MnAs layer, mediating a direct ferromagnetic interaction between Mn atoms.


第5回三機関連携「量子複雑現象; 超伝導と磁性とフォノン」研究会講演集

社本 真一; 樹神 克明

JAEA-Review 2012-029, 264 Pages, 2012/08




Dynamical spin susceptibility studied by inelastic neutron scattering on LaFeAsO$$_{1-x}$$F$$_{x}$$

社本 真一; 石角 元志; 脇本 秀一; 樹神 克明; 梶本 亮一; 新井 正敏

Journal of Physics; Conference Series, 340, p.012075_1 - 012075_6, 2012/02

 被引用回数:1 パーセンタイル:48.68

Low-energy spin excitations on polycrystalline LaFeAsO$$_{1-x}$$F$$_{x}$$ samples have been studied by inelastic neutron scattering. The $$Q$$-integrated dynamical spin susceptibility $$chi$$"($$omega$$) at 11 meV decreases with increasing fluorine content $$x$$ across the phase transition from antiferromagnetic to superconducting phases. For superconducting samples, a peak in $$chi$$"($$omega$$) develops at $$omega$$ = $$E$$$$_{rm res}$$ below $$T$$$$_{rm c}$$, accompanied by its reduction below $$E$$$$_{rm res}$$. Fe 3$$d$$ orbital contribution on the dynamical spin susceptibility and the electron scattering between $$Gamma$$and $$M$$ Fermi surfaces are discussed.

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