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門野 良典*; 伊藤 孝
Journal of the Physical Society of Japan, 94(6), p.064601_1 - 064601_11, 2025/06
We extend the previously published model that distinguishes between the diffusive motion of diamagnetic muons and the dynamics of ions around the muon in matter, and propose a generalized model for 
(Mu
s, bound states of a muon and an unpaired electron) observed in non-metallic host materials. The new model distinguishes among the independent motion of unpaired electron associated with Mu, the self-diffusive motion of Mu as single atomic entity, and that of the ions surrounding Mu, where the muon spin relaxation is induced by dynamical fluctuations of the hyperfine (HF) field exerted from the unpaired electron (e.g., due to spin/charge exchange reaction) and/or that of the nuclear hyperfine (NHF) interactions between the unpaired electron and the surrounding ions. We have applied this model to the muonated radicals (Mus in a polaron state) in conducting polymers, and examined the validity of the interpretations claimed in the earlier literature that the spin relaxation is induced by quasi-one dimensional jump motion of the unpaired electron. The result suggests that experimental support for such a claim is still inadequate and needs to be reexamined, including the possibility of other origins for the fluctuations. It is expected that our model will prove a useful guide for 
SR studies of various local dynamics involving paramagnetic muon states.
Co
)Sn studied by SRCai, Y.*; Yoon, S.*; Sheng, Q.*; Zhao, G.*; Seewald, E. F.*; Ghosh, S.*; Ingham, J.*; Pasupathy, A. N.*; Queiroz, R.*; Lei, H.*; et al.
Physical Review B, 111(21), p.214412_1 - 214412_17, 2025/06
We study the magnetic properties of the metallic kagome system (FeCo)Sn by a combination of muon spin relaxation (SR), magnetic susceptibility, and scanning tunneling microscopy (STM) measurements in single crystal specimens with Co concentrations 
= 0, 0.11, 0.8. In the undoped antiferromagnetic compound FeSn, we find possible signatures for a previously unidentified phase that sets in at 
~K, well beneath the Neel temperature 
~K as indicated by a peak in the relaxation rate 1/
observed in zero field (ZF) and longitudinal field (LF) SR measurements, with a corresponding anomaly in the ac and dc susceptibility, and an increase in the static width 1/
in ZF-SR measurements. No signatures of spatial symmetry breaking are found in STM down to 7~K. Related to the location and motion of muons in FeSn, we confirmed a previous report that about 40% of the implanted muons reside at a field-cancelling high symmetry site at 
~K, while an onset of thermal hopping changes the site occupancy at higher temperatures. In Fe
Co
Sn, where disorder eliminated the field-cancellation effect, all the implanted muons exhibit precession and/or relaxation in the ordered state. In Fe
Co
Sn, we find canonical spin glass behavior with freezing temperature 
~K; the ZF and LF-SR time spectra exhibit results similar to those observed in dilute alloy spin glasses CuMn and AuFe, with a critical behavior of 
at 
and 
as 
. The absence of spin dynamics at low temperatures makes a clear contrast to the spin dynamics observed by SR in many geometrically frustrated spin systems on insulating kagome, pyrochlore, and triangular lattices. The spin glass behavior of CoSn doped with dilute Fe moments is shown to originate primarily from the randomness of doped Fe moments rather than due to geometrical frustration of the underlying lattice.
SRによるイオンダイナミクス解析の精密化に向けた動的久保-鳥谷部モデルの拡張伊藤 孝; 門野 良典*
固体物理, 60(4), p.197 - 206, 2025/04
SRを用いた固体内イオンダイナミクス解析法が抱える深刻な矛盾を解消するために、その根幹をなす動的久保・鳥谷部モデルの拡張を試みた。我々の新しいモデルは、ミュオン静止描像の上での定量的な解析を可能にするだけでなく、この前提の妥当性を評価する手段を同時に提供する。
Sb with a honeycomb network足立 匡*; Ogawa, Taiki*; 小宮山 陽太*; 須村 拓也*; Saito-Tsuboi, Yuki*; Takeuchi, Takaaki*; Mano, Kohei*; Manabe, Kaoru*; 川端 幸樹*; 今津 毅士*; et al.
Physical Review B, 111(10), p.L100508_1 - L100508_6, 2025/03
被引用回数：0 パーセンタイル：0.00(Materials Science, Multidisciplinary)Chiral superconductivity exhibits the formation of novel electron pairs that breaks the time-reversal symmetry and has been actively studied in various quantum materials in recent years. However, despite its potential to provide definitive information, effects of disorder in the crystal structure on the chiral superconductivity has not yet been clarified, and therefore the investigation using a solid-solution system is desirable. We report muon-spin-relaxation (SR) results of layered pnictide BaPtAsSb with a honeycomb network composed of Pt and (As, Sb). We observed an increase of the zero-field SR rate in the superconducting (SC) state at the Sb end of 
, suggesting the occurrence of a spontaneous magnetic field due to the time-reversal symmetry breaking in the SC state. On the other hand, a spontaneous magnetic field was almost and completely suppressed for the As-Sb mixed samples of 
and 0.2, respectively, suggesting that the time-reversal symmetry-breaking SC state in is sensitive to disorder. The magnetic penetration depth estimated from transverse-field SR measurements at and 0.2 behaved like weak-coupling 
-wave superconductivity. These seemingly incompatible zero-field and transverse-field SR results of BaPtAsSb with could be understood in terms of chiral 
-wave superconductivity with point nodes on the three-dimensional Fermi surface.
Sm synchrotron-radiation-based M
ssbauer and 
SR studies of Sm
Ru
Ge
筒井 智嗣; 伊藤 孝; 中村 仁*; 吉田 実生*; 小林 義男*; 依田 芳卓*; 中村 惇平*; 幸田 章宏*; 東中 隆二*; 青木 大*; et al.
Interactions (Internet), 245(1), p.55_1 - 55_9, 2024/12
Sm SR-based Mssbauer and muon spin relaxation (SR) spectroscopies have been applied to SmRuGe. The temperature dependence of the Sm SR-based Mssbauer spectra in the paramagnetic state implies the presence of dynamical nuclear Zeeman and/or quadrupole interactions. The time differential SR spectra also exhibit a marked temperature dependence in the paramagnetic state, indicating the presence of magnetic fluctuation in SmRuGe at least. These results in the present work infer that the dynamical hyperfine interactions observed using the mutually complementary spectroscopic methods are connected with the mechanism of the heavy fermion behavior in SmRuGe.
下村 浩一郎*; 幸田 章宏*; Pant, A. D.*; 砂川 光*; 藤森 寛*; 梅垣 いづみ*; 中村 惇平*; 藤原 理賀; 反保 元伸*; 河村 成肇*; et al.
Interactions (Internet), 245(1), p.31_1 - 31_6, 2024/12
J-PARC Muon Facility: MUSE (Muon Science Establishment) is responsible for the inter-university user program and the operation, maintenance, and construction of the muon beamlines, namely D-line, S-line, U-line, and H-line, along with the muon source at J-PARC Materials and Life Science Facility (MLF). In this paper, recent developments are briefly presented.
)(SrAl
TaO) with 
伊藤 孝; 髭本 亘; 幸田 章宏*; 中村 惇平*; 下村 浩一郎*
Interactions (Internet), 245(1), p.25_1 - 25_7, 2024/12
We report on muon spin relaxation (SR) measurements in a mixed perovskite compound, (LaAlO)
(SrAlTaO) with (LSAT), which is widely used as a single-crystalline substrate for thin film deposition. In zero applied field (ZF), muon depolarization due to the distribution of nuclear dipole fields was observed in the temperature range from 4 K to 270 K. Interestingly, SR time spectra in ZF maintained a Gaussian-like feature over the entire range, while the depolarization rate exhibited a monotonic decrease with increasing temperature. This behavior may be attributed to the thermally activated diffusion of muons between a few adjacent sites within a confined space of the angstrom scale, where the motionally averaged local field that each muon experiences can remain non-zero and result in maintaining the Gaussian-like line shape. The spatial distribution of electrostatic potential at lattice interstices evaluated via density functional theory calculations suggests that such a restriction of muon diffusion paths can be caused by the random distribution of cations with different nominal valences in the mixed perovskite lattice.
Sm synchrotron-radiation-based Mssbauer spectroscopy of Sm-based heavy fermion compounds筒井 智嗣; 東中 隆二*; 水牧 仁一朗*; 小林 義男*; 中村 仁*; 伊藤 孝; 依田 芳卓*; 松田 達磨*; 青木 勇二*; 佐藤 英行*
Interactions (Internet), 245(1), p.9_1 - 9_10, 2024/12
Sm synchrotron-radiation-based Mssbauer spectroscopy has been applied to Sm-based heavy fermion intermetallics, Sm
Al
(
= Ti, V and Cr) and SmOs
Sb
. The isomer shifts obtained demonstrate that the Sm valence states in these compounds are intermediate. Since the difference of the isomer shifts in 22.502 keV Sm Mssbauer effect between Sm
and Sm
state is comparable to the 2nd order Doppler shift, consideration of the 2nd order Doppler shift is required to precisely discuss Sm valence state through the shifts of the Mssbauer spectra. In addition, the plots of the isomer shifts obtained by the Mssbauer spectroscopy against the Sm valence states estimated from Sm L-edge X-ray absorption spectroscopy exhibit a linear correlation except for that in SmOsSb. This implies that the origin of the intermediate valence state in SmOsSb differs from that in SmAl ( = Ti, V and Cr).
SR study on the noncentrosymmetric superconductor NbGe
Jiao, J. C.*; Chen, K. W.*; Hillier, A. D.*; 伊藤 孝; 髭本 亘; Li, Z.*; Lv, B.*; Xu, Z.-A.*; Shu, L.*
Physical Review B, 110(21), p.214516_1 - 214516_9, 2024/12
被引用回数：0 パーセンタイル：0.00(Materials Science, Multidisciplinary)We report on a muon spin relaxation (SR) study on the polycrystalline noncentrosymmetric superconductor NbGe with superconducting transition temperature 
= 2.0-2.1 K. The zero-field SR experiment indicates the absence of a spontaneous magnetic field in the superconducting state, showing the preservation of time-reversal symmetry in the superconducting state. The transverse-field SR experiment is performed to map the phase diagram of NbGe, from which clear evidence of both type-I and type-II superconductivities is obtained. More importantly, we clearly delineate the region in the phase diagram where type-I and type-II superconductivities coexist.
二宮 和彦*; 久保 謙哉*; 稲垣 誠*; 吉田 剛*; 竹下 聡史*; 反保 元伸*; 下村 浩一郎*; 河村 成肇*; Strasser, P.*; 三宅 康博*; et al.
Journal of Radioanalytical and Nuclear Chemistry, 333(7), p.3445 - 3450, 2024/07
被引用回数：1 パーセンタイル：57.00(Chemistry, Analytical)A novel nondestructive light element analysis method for bulk materials using muon beams was demonstrated. This method is based on the lifetime measurement of muons in a material and performed by measuring muon-decay electrons and identifying elements using the atomic number based on muon lifetimes. Muon irradiation on pure iron and two steel samples with known carbon contents was conducted to prepare a calibration curve for the quantitative analysis. We also performed a muon lifetime measurement for a Japanese sword and successfully determined its carbon content as 0.51 wt% using the calibration curve, without sample destruction.
伊藤 孝; 門野 良典*
Journal of the Physical Society of Japan, 93(4), p.044602_1 - 044602_7, 2024/04
被引用回数：3 パーセンタイル：68.78(Physics, Multidisciplinary)We propose a model to describe the fluctuations in the internal magnetic field due to ion dynamics observed in muon spin relaxation (SR) by an Edwards-Anderson-type autocorrelation function that separates the quasi-static and dynamic components of the correlation by the parameter 
(where 
). Our Monte Carlo simulations for this model showed that the time evolution of muon spin polarization deviates significantly from the Kubo-Toyabe function. To further validate the model, the results of simulations were compared with the SR spectra observed in a hybrid organic-inorganic perovskite FAPbI [with FA referring to HC(NH)], where local field fluctuations associated with the rotational motion of FA molecules and quasi-static fields from the PbI lattice are presumed to coexist. The least-squares curve fitting showed reasonable agreement with the model with 
, and the fluctuation frequency of the dynamical component was obtained. This result opens the door to the possibility of experimentally distinguishing fluctuations due to the dynamics of ions around muons from those due to the self-diffusion of muons. On the other hand, it suggests the need to carefully consider the spin relaxation function when applying SR to the issue of ion dynamics.
池田 一貴*; 佐次田 頌*; 大友 季哉*; 大下 英敏*; 本田 孝志*; 羽合 孝文*; 齋藤 開*; 伊藤 晋一*; 横尾 哲也*; 榊 浩司*; et al.
International Journal of Hydrogen Energy, 51(Part A), p.79 - 87, 2024/01
被引用回数：6 パーセンタイル：48.53(Chemistry, Physical)Low-vanadium-concentration alloys have low durability, and their hydrogen absorption and desorption amounts decrease by 20% after 100 cycles. In this study, we conducted reverse Monte Carlo modeling on X-ray diffraction patterns and neutron pair distribution functions of the hydrogen-absorbed and desorbed samples of a V
Ti
Cr
alloy to analyze the variations in the local structure. The local structure surrounding the hydrogen atom in the hydrogen-absorbed phase exhibited minimal changes. In contrast, hydrogen occupied both tetrahedral and octahedral sites of the hydrogen-desorbed phase almost equally during the early cycles; however, the amount of hydrogen occupying the tetrahedral sites increased with the number of cycles.
二宮 和彦*; 久保 謙哉*; 稲垣 誠*; 吉田 剛*; Chiu, I.-H.; 工藤 拓人*; 浅利 駿介*; 千徳 佐和子*; 竹下 聡史*; 下村 浩一郎*; et al.
Scientific Reports (Internet), 14, p.1797_1 - 1797_8, 2024/01
被引用回数：0 パーセンタイル：0.00(Multidisciplinary Sciences)鋼の特性を決める上で重要な鋼中のC量は、鋼の生産技術に大きく左右される。このため、ミュオンを使って鋼のC含有量を非破壊で測定する新しい方法を提案する。この方法は、生産中の鋼の品質管理だけでなく、貴重な鋼製考古学的遺物の分析にも使えるかもしれない。負の電荷を持つミュオンは原子系を形成し、最終的には核に吸収されるか電子に崩壊する。ミュオンの寿命は、Fe原子かC原子に捕らわれるかによってかなり違い、ミュオン停止位置での元素含有量をミュオン寿命測定で特定できる。C/Feのミュオン捕獲確率とCの元素含有量の関係は直線的で、ミュオン寿命測定で鋼のC含有量を定量的に決められる。さらに、ミュオンの入射エネルギーを調整して、0.5mm厚の3種類の鋼板からなる積層サンプルの各層でミュオンを停止させ、0.20-1.03wt%の範囲でC含有量を深さ選択的に、サンプルを壊さずに決定することに成功した。
伊藤 孝; 髭本 亘; 下村 浩一郎*
Physical Review B, 108(22), p.224301_1 - 224301_11, 2023/12
被引用回数：6 パーセンタイル：58.52(Materials Science, Multidisciplinary)In positive muon spin rotation and relaxation (SR) spectroscopy, positive muons () implanted into solid oxides are conventionally treated as immobile spin-probes at interstitial sites below room temperature. This is because each is thought to be tightly bound to an oxygen atom in the host lattice to form a muonic analogue of the hydroxy group. On the basis of this concept, anomalies in SR spectra observed in oxides have been attributed in most cases to the intrinsic properties of host materials. On the other hand, global diffusion with an activation energy of 
0.1~eV has been reported in some chemically-substituted perovskite oxides at cryogenic temperatures, although the reason for the small activation energy despite the formation of the strong O bond has not yet been quantitatively understood. In this study, we investigated interstitial diffusion in the perovskite oxide lattice using KTaO cubic perovskite as a model system. We used the SR method and density functional theory calculations along with the harmonic transition state theory to study this phenomenon both experimentally and theoretically. Experimental activation energies for global diffusion obtained below room temperature were less than a quarter of the calculated classical potential barrier height for a bottleneck transfer path. The reduction in the effective barrier height could be explained by the harmonic transition state theory with a zero-point energy correction; a significant difference in zero-point energies for at the positions in the O bonding equilibrium state and a bond-breaking transition state was the primary cause of the reduction. This suggests that the assumption of immobile in solid oxides is not always satisfied since such a significant decrease in diffusion barrier height can also occur in other oxides.
美崎 慧*; 三輪 寛子*; 伊藤 孝; 吉田 健文*; 長谷川 慎吾*; 中村 由紀奈*; 徳竹 駿太*; 高畠 萌*; 下村 浩一郎*; Chun, W.-J.*; et al.
ACS Catalysis, 13(18), p.12281 - 12287, 2023/09
被引用回数：6 パーセンタイル：48.53(Chemistry, Physical)The direct alkylation of benzenes with simple alkanes is one of the ideal processes for the production of alkylbenzenes. We demonstrated that Pd nanoparticles on the outer surface of H-ZSM-5 are efficient catalysts for direct alkylation. The reaction proceeds through the activation of an alkane on the acid sites present inside the zeolite pores. This process is followed by the nucleophilic addition of an arene to the activated alkane. The spillover of the abstracted hydrogen atoms from the acid sites to the Pd nanoparticles on the outer surface accelerates recombination to H. A maximum toluene conversion of 58.5% and selectivity of 95.6% for the alkylated products are achieved when toluene is reacted with 
-heptane. 
-selective alkylation is achieved, due to the effect of the pore size of H-ZSM-5. The SR study of muonium, a pseudo-isotope of hydrogen, in aluminosilicates suggested that the formation of atomic hydrogen is possible and its lifetime is in the sub-microsecond range or longer, which is long enough for chemical reactions.
寺澤 知潮; 松永 和也*; 林 直輝*; 伊藤 孝寛*; 田中 慎一郎*; 保田 諭; 朝岡 秀人
Vacuum and Surface Science, 66(9), p.525 - 530, 2023/09
Au(001)表面は擬一次元周期性を持つHex-Au(001)に再構成することから、この表面にグラフェンを成長させると、その周期性がグラフェンの電子構造を変化させると予測された。特に、グラフェンとAuの軌道混成により、グラフェンにバンドギャップやスピン偏極が導入されると考えられていた。本研究では、Hex-Au(001)表面上のグラフェンの角度分解光電子分光と密度汎関数理論計算の結果を報告する。グラフェンのDiracコーンとAu 6sp軌道の交点に0.2eVのバンドギャップが観測され、バンドギャップ形成の起源がグラフェンのDiracコーンとAu 6sp軌道の混成であることが示された。この軌道混成の機構について考察し、グラフェンのDiracコーンへのスピン注入を予想した。
inferred from muon study門野 良典*; 平石 雅俊*; 岡部 博孝*; 幸田 章宏*; 伊藤 孝
Journal of Physics; Condensed Matter, 35(28), p.285503_1 - 285503_13, 2023/07
被引用回数：1 パーセンタイル：11.20(Physics, Condensed Matter)Magnesium hydride has great potential as a solid hydrogen (H) storage material because of its high H storage capacity of 7.6 wt%. However, its slow hydrogenation and dehydrogenation kinetics and the high temperature of 300 
C required for decomposition are major obstacles to small-scale applications such as automobiles. The local electronic structure of interstitial H in MgH is an important fundamental knowledge in solving this problem, which has been studied mainly based on density functional theory (DFT). However, few experimental studies have been performed to assess the results of DFT calculations. We have therefore introduced muon (Mu) as pseudo-H into MgH and investigated the corresponding interstitial H states by analyzing their electronic and dynamical properties in detail. As a result, we observed multiple Mu states similar to those observed in wide-gap oxides, and found that their electronic states can be attributed to relaxed-excited states associated with donor/acceptor levels predicted by the recently proposed ambipolarity model. This provides an indirect support for the DFT calculations on which the model is based via the donor/acceptor levels. An important implication of the muon results for improved hydrogen kinetics is that dehydrogenation, serving as a reduction for hydrides, stabilises the interstitial H
state.
SR) methods伊藤 孝; 下村 浩一郎*
Hydrogenomics; The Science of Fully Utilizing Hydrogen (Internet), p.43 - 49, 2023/03
A brief introduction to the muon spin rotation, relaxation, and resonance (SR) methods is given for researchers and students involved in hydrogen science research. The text includes several examples of how the SR methods can be used to elucidate the behavior of hydrogen in materials.
下村 浩一郎*; 幸田 章宏*; Pant, A. D.*; 名取 寛顕*; 藤森 寛*; 梅垣 いづみ*; 中村 惇平*; 反保 元伸*; 河村 成肇*; 手島 菜月*; et al.
Journal of Physics; Conference Series, 2462, p.012033_1 - 012033_5, 2023/03
被引用回数：0 パーセンタイル：0.00(Physics, Applied)At J-PARC MUSE, since the SR2017 conference and up to FY2022, there have been several new developments at the facility, including the completion of a new experimental area S2 at the surface muon beamline S-line and the first muon beam extraction to the H1 area in the H-line, mainly to carry out high-statistics fundamental physics experiments. Several new studies are also underway, such as applying negative muon non-destructive elemental analysis to the analysis of samples returned from the asteroid Ryugu in the D2 area of the D-line. This paper reports on the latest status of MUSE.
Zn probed by muon spin relaxation髭本 亘; 佐藤 一彦*; 伊藤 孝; 大石 一城*; 才賀 裕太*; 小坂 昌史*; 松林 和幸*; 上床 美也*
Journal of Physics; Conference Series, 2462, p.012039_1 - 012039_5, 2023/03
被引用回数：0 パーセンタイル：0.00(Physics, Applied)立方晶構造を持つYbCoZnは極めて大きい電子比熱係数を持つことが知られ、またその基底状態は量子臨界点の近傍に位置するものと考えられている。実際に1-2GPaの圧力をかけると長距離磁気秩序状態が確認されている。我々はこの物質の常圧での磁気的基底状態を確認するためにミュオンスピン緩和測定を行った。その結果小さな磁気モーメントが作る揺らいだ磁場が観測された。
