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Temporally decoherent and spatially coherent vibrations in metal halide perovskites

Zhang, D.*; Hu, X.*; Chen, T.*; Abernathy, D. L.*; 梶本 亮一; 中村 充孝; 古府 麻衣子; Foley, B. J.*; Yoon, M.*; Choi, J. J.*; et al.

Physical Review B, 102(22), p.224310_1 - 224310_10, 2020/12

The long carrier lifetime and defect tolerance in metal halide perovskites (MHPs) are major contributors to the superb performance of MHP optoelectronic devices. Large polarons were reported to be responsible for the long carrier lifetime. Yet microscopic mechanisms of the large polaron formation, including the so-called phonon melting, are still under debate. Here, time-of-flight inelastic neutron scattering experiments and first-principles density-functional theory calculations were employed to investigate the lattice vibrations (or phonon dynamics) in methylammonium lead iodide, a prototypical example of MHPs. Our findings are that optical phonons lose temporal coherence gradually with increasing temperature which vanishes at the orthorhombic-to-tetragonal structural phase transition. Surprisingly, however, we found that the spatial coherence is still retained throughout the decoherence process. We argue that the temporally decoherent and spatially coherent vibrations contribute to the formation of large polarons in this metal halide perovskite.


Coexistence of two components in magnetic excitations of La$$_{2-x}$$Sr$$_{x}$$CuO$$_{4}$$ ($$x$$ = 0.10 and 0.16)

佐藤 研太朗*; 池内 和彦*; 梶本 亮一; 脇本 秀一; 新井 正敏*; 藤田 全基*

Journal of the Physical Society of Japan, 89(11), p.114703_1 - 114703_7, 2020/11


To elucidate the spin dynamics of La$$_{2-x}$$Sr$$_{x}$$CuO$$_{4}$$, which couples with the charge degree of freedom, the spin excitations spanning the characteristic energy ($$E_mathrm{cross}$$ $$sim$$ 35--40 meV) are investigated for underdoped $$x$$ = 0.10 and optimally doped (OP) $$x$$ = 0.16 through inelastic neutron scattering measurements. Analysis based on a two-component picture of high-quality data clarified the possible coexistence of upright standing incommensurate (IC) excitations with gapless commensurate (C) excitations in the energy-momentum space. The IC component weakens the intensity toward $$E_mathrm{cross}$$ with increasing energy transfer ($$hbaromega$$), whereas the C component strengthens at high-$$hbaromega$$ regions. The analysis results imply that the superposition of two components with a particular intensity balance forms an hourglass-shaped excitation in appearance. Furthermore, the temperature dependence of the intensity of each component exhibits different behaviors; the IC component disappears near the pseudo-gap temperature ($$T^*$$) upon warming, whereas the C component is robust against temperature. These results suggest the itinerant electron spin nature and the localized magnetism of the parent La$$_{2}$$CuO$$_{4}$$ in IC and C excitations, respectively, similar to the spin excitations in the OP YBa$$_{2}$$Cu$$_{3}$$O$$_{6+delta}$$ and HgBa$$_{2}$$CuO$$_{4+delta}$$ with higher superconducting-transition temperatures.


Energy resolution and neutron flux of the 4SEASONS spectrometer revisited

梶本 亮一; 中村 充孝; 飯田 一樹*; 蒲沢 和也*; 池内 和彦*; 稲村 泰弘; 石角 元志*

Journal of Neutron Research, 22(2-3), p.99 - 107, 2020/10

The elastic energy resolution, integrated intensity, and peak intensity of the direct-geometry neutron chopper spectrometer 4SEASONS at Japan Proton Accelerator Research Complex (J-PARC) were re-investigated. This was done with respect to the incident energy and the rotation speed of the Fermi chopper using incoherent scattering of vanadium and simple analytical formulas. The model calculations reproduced the observed values satisfactorily. The present work should be useful for estimating in instrument performance in experiments.


Structural, magnetic, transport, and thermoelectric properties of the pseudobrookite AlTi$$_{2}$$O$$_{5}$$-Ti$$_{3}$$O$$_{5}$$ system

高濱 隆成*; 石井 透依*; 犬童 代梧*; 有薗 実駿*; 寺倉 千恵子*; 十倉 好紀*; 竹下 直*; 野田 正亮*; 桑原 英樹*; 斎木 琢夫*; et al.

Physical Review Materials (Internet), 4(7), p.074401_1 - 074401_11, 2020/07

 被引用回数:0 パーセンタイル:100(Materials Science, Multidisciplinary)

We investigated the structural, magnetic, transport, and high-temperature thermoelectric properties of single crystals of the pseudobrookite Al$$_{1-x}$$Ti$$_{2+x}$$O$$_{5}$$ for $$0 le x le 1$$ grown using a floating zone. We found a correlation of spin-singlet Ti$$^{3+}$$-Ti$$^{3+}$$ dimers coupled with the lattice even in the conductive $$alpha$$ and $$lambda$$ phases which develops with increasing $$x$$. This developing dimer correlation reduces the number of unpaired Ti$$^{3+}$$ ions, which makes the compound more conductive owing to the suppression of disorder for $$x$$ up to about 0.75. The dimer fluctuation causes a critical enhancement of the magnetic susceptibility at around 150 K in the $$lambda$$ phase near the boundary ($$x sim 0.9$$) between the $$lambda$$ and the $$beta$$ phases. Such a correlation of the spin-singlet Ti$$^{3+}$$-Ti$$^{3+}$$ dimers may produce a high Seebeck coefficient in the conductive $$alpha$$ and $$lambda$$ phases leading to a large thermoelectric power factor at high temperatures.


Evidence for magnon-phonon coupling in the topological magnet Cu$$_{3}$$TeO$$_{6}$$

Bao, S.*; Cai, Z.*; Si, W.*; Wang, W.*; Wang, X.*; Shangguan, Y.*; Ma, Z.*; Dong, Z.-Y.*; 梶本 亮一; 池内 和彦*; et al.

Physical Review B, 101(21), p.214419_1 - 214419_8, 2020/06

 被引用回数:0 パーセンタイル:100(Materials Science, Multidisciplinary)

We perform thermodynamic and inelastic neutron scattering (INS) measurements to study the lattice dynamics (phonons) of a cubic collinear antiferromagnet Cu$$_{3}$$TeO$$_{6}$$ which hosts topological spin excitations (magnons). While the specific heat and thermal conductivity results show that the thermal transport is dominated by phonons, the deviation of the thermal conductivity from a pure phononic model indicates that there is a strong coupling between magnons and phonons. In the INS measurements, we find a mode in the excitation spectra at 4.5 K, which exhibits a slight downward dispersion around the Brillouin zone center. This mode disappears above the N$'{e}$el temperature and thus cannot be a phonon. Furthermore, the dispersion is distinct from that of a magnon. Instead, it can be explained by the magnon-polaron mode, collective excitations resulting from the hybridization between magnons and phonons. We consider the suppression of the thermal conductivity and emergence of the magnon-polaron mode to be evidence for magnon-phonon coupling in Cu$$_{3}$$TeO$$_{6}$$.


Horizontal line nodes in Sr$$_2$$RuO$$_4$$ proved by spin resonance

飯田 一樹*; 古府 麻衣子; 鈴木 雄大*; 村井 直樹; 河村 聖子; 梶本 亮一; 稲村 泰弘; 石角 元志*; 長谷川 舜介*; 増田 隆嗣*; et al.

Journal of the Physical Society of Japan, 89(5), p.053702_1 - 053702_5, 2020/05

 被引用回数:2 パーセンタイル:14.51(Physics, Multidisciplinary)

We investigated the low-energy incommensurate (IC) magnetic fluctuations in Sr$$_2$$RuO$$_4$$ by the high-resolution inelastic neutron scattering measurements and random phase approximation (RPA) calculations. We observed a spin resonance with energy of $$hbar omega_{rm res}0.56$$ meV centered at a characteristic wavevector $$Q_{rm res}=(0.3,0.3,0.5)$$. The resonance energy corresponds well to the superconducting gap 2$$Delta$$ = 0.56 meV estimated by the tunneling spectroscopy. The spin resonance shows the $$L$$ modulation with a maximum at around $$L = 0.5$$. The $$L$$ modulated intensity of the spin resonance and our RPA calculations indicate that the superconducting gaps regarding the quasi-one-dimensional $$alpha$$ and $$beta$$ sheets at the Fermi surfaces have the horizontal line nodes. These results may set a strong constraint on the pairing symmetry of Sr$$_2$$RuO$$_4$$. We also discuss the implications on possible superconducting order parameters.


The $$f$$-electron state of the heavy fermion superconductor NpPd$$_5$$Al$$_2$$ and the isostructural family

目時 直人; Aczel, A. A.*; 青木 大*; Chi, S.*; Fernandez-Baca, J. A.*; Griveau, J.-C.*; 萩原 正人*; Hong, T.*; 芳賀 芳範; 池内 和彦*; et al.

JPS Conference Proceedings (Internet), 30, p.011123_1 - 011123_6, 2020/03



Strong local moment antiferromagnetic spin fluctuations in V-doped LiFeAs

Xu, Z.*; Dai, G.*; Li, Y.*; Yin, Z.*; Rong, Y.*; Tian, L.*; Liu, P.*; Wang, H.*; Xing, L.*; Wei, Y.*; et al.

npj Quantum Materials (Internet), 5(1), p.11_1 - 11_7, 2020/02

 被引用回数:2 パーセンタイル:26.75(Materials Science, Multidisciplinary)

We use neutron scattering to study Vanadium (hole)-doped LiFe$$_{1-x}$$V$$_{x}$$As. In the undoped state, LiFeAs exhibits superconductivity at $$T_mathrm{c} = 18$$ K and transverse incommensurate spin excitations similar to electron overdoped iron pnictides. Upon Vanadium doping to form LiFe$$_{0.955}$$V$$_{0.045}$$, the transverse incommensurate spin excitations in LiFeAs transform into longitudinally elongated ones in a similar fashion to that of potassium (hole)-doped Ba$$_{0.7}$$K$$_{0.3}$$Fe$$_{2}$$As$$_{2}$$ but with dramatically enhanced magnetic scattering and elimination of superconductivity. This is different from the suppression of the overall magnetic excitations in hole-doped BaFe$$_{2}$$As$$_{2}$$ and the enhancement of superconductivity near optimal hole doping. These results are consistent with density function theory plus dynamic mean field theory calculations, suggesting that Vanadium doping in LiFeAs may induce an enlarged effective magnetic moment $$S_mathrm{eff}$$ with a spin crossover ground state arising from the inter-orbital scattering of itinerant electrons.


Experimental investigation of the suppressed superconducting gap and double-resonance mode in Ba$$_{1-x}$$K$$_{x}$$Fe$$_{2}$$As$$_{2}$$

出田 真一郎*; 村井 直樹; 中島 正道*; 梶本 亮一; 田中 清尚*

Physical Review B, 100(23), p.235135_1 - 235135_7, 2019/12

 被引用回数:0 パーセンタイル:100(Materials Science, Multidisciplinary)

Ba$$_{1-x}$$K$$_{x}$$Fe$$_{2}$$As$$_{2}$$ has an exotic physical property where that the C$$_{2}$$-SDW phase suddenly changes to the C$$_{4}$$-magnetic phase and superconductivity is suppressed within a narrow composition range around x = 0.25. We have investigated the doping dependence of the electronic structure of Ba$$_{1-x}$$K$$_{x}$$Fe$$_{2}$$As$$_{2}$$ using angle-resolved photoemission spectroscopy (ARPES) and found an anomaly in the superconducting (SC) gap structure only for x = 0.25 in both the hole and electron Fermi surfaces (FSs). We also propose that the mechanism of a newly observed double-resonance peak by inelastic neutron scattering is understandable by the SC gap obtained by ARPES. Our discovery reveals the important relationship between the C$$_{4}$$- magnetic phase and superconductivity, and provides an opportunity to survey the underlying relationship between the SC gap and resonance mode in the hole-doped iron-based superconductor.


Crystal structures of highly hole-doped layered perovskite nickelate Pr$$_{2-x}$$Sr$$_{x}$$NiO$$_{4}$$ studied by neutron diffraction

梶本 亮一; 中島 健次; 藤田 全基*; 石角 元志*; 鳥居 周輝*; 石川 喜久*; Miao, P.*; 神山 崇*

Journal of the Physical Society of Japan, 88(11), p.114602_1 - 114602_6, 2019/11

 被引用回数:0 パーセンタイル:100(Physics, Multidisciplinary)

A high-resolution time-of-flight powder neutron diffraction study of the layered nickel oxide Pr$$_{2-x}$$Sr$$_{x}$$NiO$$_{4}$$ with $$x = 0.7$$ and $$0.9$$ was performed to characterize the crystal structures of these highly hole-doped nickelates. For the sample with $$x = 0.7$$, the Ni-O bond lengths decrease uniformly with decreasing temperature, and the atomic displacement parameters are similar to those for $$x = 1/3$$. In contrast, for the sample with $$x = 0.9$$, the out-of-plane Ni-O bond length shows a sharp thermal contraction in the high-temperature region, which is suggestive of changes in the orbital occupation accompanied by the development of checkerboard-type charge correlations. Furthermore, the $$x = 0.9$$ sample is characterized by a large atomic displacement parameter for the apical O atoms along the out-of-plane direction, which is interpreted as the existence of two types of Ni$$^{3+}$$ sites with different orbital occupancies. The distinct difference between the $$x = 0.9$$ sample and the lower-concentration compounds should be related to the development of checkerboard-type charge ordering in the metallic matrix and possible orbital ordering at the Ni$$^{3+}$$ sites at $$x sim 1$$ in the hole-doped layered nickel oxides.


Q dependence of magnetic resonance mode on FeTe$$_{0.5}$$Se$$_{0.5}$$ studied by inelastic neutron scattering

石角 元志*; 樹神 克明; 梶本 亮一; 中村 充孝; 稲村 泰弘; 池内 和彦*; Ji, S.*; 新井 正敏*; 社本 真一

Condensed Matter (Internet), 4(3), p.69_1 - 69_10, 2019/09



Status of neutron spectrometers at J-PARC

梶本 亮一; 横尾 哲也*; 中村 充孝; 川北 至信; 松浦 直人*; 遠藤 仁*; 瀬戸 秀紀*; 伊藤 晋一*; 中島 健次; 河村 聖子

Physica B; Condensed Matter, 562, p.148 - 154, 2019/06

 被引用回数:3 パーセンタイル:60.07(Physics, Condensed Matter)

Seven time-of-flight quasielastic/inelastic neutron scattering instruments are installed on six beamlines in the Materials and Life Science Experimental Facility (MLF) at the Japan Proton Accelerator Research Complex (JPARC). Four of these instruments are chopper-type direct-geometry spectrometers, one is a near-backscattering indirect-geometry spectrometer, and the other two are spin-echo-type spectrometers. This paper reviews the characteristic features, recent scientific outcomes, and progress in development of MLF spectrometers.


Study on use of superconducting magnet and first inelastic neutron scattering experiment under magnetic field at 4SEASONS spectrometer

梶本 亮一; 石角 元志*; 吉良 弘*; 金子 耕士; 中村 充孝; 蒲沢 和也*; 稲村 泰弘; 池内 和彦*; 飯田 一樹*; 村井 直樹; et al.

Physica B; Condensed Matter, 556, p.26 - 30, 2019/03

 被引用回数:2 パーセンタイル:60.07(Physics, Condensed Matter)

Magnets are important for studying magnetism and are commonly used as sample environment devices of neutron scattering instruments. However, the use of magnets was prevented at the time-of-flight direct-geometry neutron spectrometer 4SEASONS in Materials and Life Science Experimental Facility (MLF) at J-PARC, because the instrument is surrounded by iron components, and it is equipped with a piece of equipment operated with magnetic bearings. In the present work, we investigate the influence of stray magnetic fields from a superconducting magnet which is shared among neutron scattering instruments in MLF. Based on the investigation, we modified 4SEASONS such that it can be used with the magnet. Finally, we successfully performed the first inelastic neutron scattering experiments with applied magnetic fields using this sample environment.



中島 健次; Harjo, S.; 山田 悟史*; 及川 健一; 梶本 亮一

JAEA-Review 2018-032, 43 Pages, 2019/02




Quantum magnetisms in uniform triangular lattices Li$$_{2}$$$$A$$Mo$$_{3}$$O$$_{8}$$ ($$A$$ = In, Sc)

飯田 一樹*; 吉田 紘行*; 岡部 博孝*; 片山 尚幸*; 石井 裕人*; 幸田 章宏*; 稲村 泰弘; 村井 直樹; 石角 元志*; 門野 良典*; et al.

Scientific Reports (Internet), 9(1), p.1826_1 - 1826_9, 2019/02

 被引用回数:1 パーセンタイル:65.14(Multidisciplinary Sciences)

Molecular based spin-1/2 triangular lattice systems have attracted research interest. Li$$_2$$$$A$$Mo$$_3$$O$$_8$$ ($$A$$ = In or Sc) is such a compound where spin-1/2 Mo$$_3$$O$$_{13}$$ clusters in place of Mo ions form the uniform triangular lattice. Here, we report exotic magnetisms in Li$$_2$$InMo$$_3$$O$$_8$$ and Li$$_2$$ScMo$$_3$$O$$_8$$ investigated by muon spin rotation ($$mu$$SR) and inelastic neutron scattering (INS) spectroscopies. Li$$_2$$InMo$$_3$$O$$_8$$ exhibits spin wave excitation which is quantitatively described by the nearest neighbor anisotropic Heisenberg model based on the 120$$^{circ}$$ spin structure. In contrast, Li$$_2$$ScMo$$_3$$O$$_8$$ undergoes short-range magnetic order below 4 K with quantum-spin-liquid-like magnetic fluctuations down to the base temperature. Origin of the different ground states is discussed in terms of anisotropies of crystal structures and magnetic interactions.


Proceedings of the User Group Meeting on MLF Spectrometers (DIRECTION 2018); October 11, 2018, Ibaraki Quantum Beam Research Center (Tokai, Ibaraki, Japan)

梶本 亮一; 横尾 哲也*; 松浦 直人*

JAEA-Review 2018-024, 78 Pages, 2019/01


平成30年10月11日、MLF中性子分光器による合同のユーザーミーティング「DIRECTION 2018」がJ-PARC MLF、高エネルギー加速器研究機構物質構造科学研究所、総合科学研究機構の共催で開催された。本ミーティングは6つの分光器、すなわちBL01(4SEASONS)、BL02(DNA)、BL06(VIN ROSE)、BL12(HRC)、BL14(AMATERAS)、BL23(POLANO)におけるユーザー利用の活性化およびユーザーと装置の協力関係の構築を目指して開催されたものである。研究会では14件の口頭発表および21件のポスター発表が行われ、各装置を利用して行われた研究成果の紹介、各装置や試料環境に関する現状の報告がなされるとともに、装置や試料環境に関する要望や今後の展開等について密接な議論が交わされた。本報告書はこのミーティングの講演要旨および講演で使用された発表資料を収録したものである。


High-energy magnetic excitations in lightly oxygen-doped lanthanum nickel oxides

中島 健次; 梶本 亮一

Physica B; Condensed Matter, 551, p.142 - 145, 2018/12

 被引用回数:0 パーセンタイル:100(Physics, Condensed Matter)

We will report on magnetic excitations in lightly oxygen doped lanthanum nickel oxide, La$$_{2}$$NiO$$_{4+delta}$$. By introducing slightly excessive oxygen atoms in the system, magnetic excitations in La$$_{2}$$NiO$$_{4}$$ drastically changes its picture. In lower energy region, spin-wave stiffness strongly suppressed. On the other hand, in the higher energy region, spin-wave dispersion curve is almost same as in the stoichiometric system, while excitations show considerable broadening. Alternation of the character of the excitations by changing energy is also reported in hole doped cuprates and cobalates. We consider that this behavior is one of key clues to understand magnetism and transport properties in carrier doped layered transition metal oxides. We investigated detail of magnetic excitations in two different lightly doped systems, La$$_{2}$$NiO$$_{4.02}$$ and La$$_{2}$$NiO$$_{4.11}$$ in wide momentum and energy transfer space by using time-of-flight spectrometers at J-PARC. Observed doping effects in magnetic excitations will be discussed by comparing them to those reported in other related layered transition metal oxides.


Performances of oscillating radial collimator for the Fermi chopper spectrometer 4SEASONS at J-PARC

中村 充孝; 神原 理*; 飯田 一樹*; 梶本 亮一; 蒲沢 和也*; 池内 和彦*; 石角 元志*; 青山 和弘*

Physica B; Condensed Matter, 551, p.480 - 483, 2018/12

 被引用回数:1 パーセンタイル:87.78(Physics, Condensed Matter)



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

 被引用回数:2 パーセンタイル:61.53(Multidisciplinary Sciences)



Al-impurity-induced magnetic excitations in heavily over-doped La$$_{1.7}$$Sr$$_{0.3}$$Cu$$_{0.95}$$Al$$_{0.05}$$O$$_{4}$$

池内 和彦*; 中島 健次; 河村 聖子; 梶本 亮一; 脇本 秀一; 鈴木 謙介*; 藤田 全基*

AIP Advances (Internet), 8(10), p.101318_1 - 101318_5, 2018/10

 被引用回数:0 パーセンタイル:100(Nanoscience & Nanotechnology)


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