arXiv subjects

H. Okabe

Publications and source records attributed to H. Okabe.

At least 19 recordsLinked to original sources

arXiv2026

Local electronic structure and dynamics of hydrogen in $\text{CeO}_2$

The local electronic states of muon (Mu) as an isotope of hydrogen (H) in high-quality single-crystalline ceria (CeO$_2$) are investigated using muon spin rotation/relaxation ($\mu\text{SR}$) and first-principles density functional theory (DFT) calculations. Upon positive muon implantation, both paramagnetic (Mu$^0$) and diamagnetic (Mu$^*$) states are observed below $\approx$10 K. Magnetic field dependence of the Mu$^0$ signals combined with DFT results provides evidence for the formation of a polaron state, consisting of Mu bonded to a ligand oxygen and a $4f$ electron localized on a nearby Ce site. The crystal-orientation dependence of the Mu$^0$ signal suggests strong anisotropy of the $4f$ electron due to the spin-orbit coupling with lifted degeneracy. Furthermore, the Mu$^0$ state exhibits transition to the Mu$^*$ state that corresponds to another Mu$^0$ state (exhibiting a diamagnetic response due to fast spin/charge fluctuations) at temperatures above $\approx$10 K, before disappearing above $\approx$30 K. These findings suggest rapid diffusive motion of the $4f$ electrons and/or Mu (as well as H) at higher temperatures.

cond-mat.mtrl-sci↗

arXiv2026

Relationship between local hydride ion dynamics and ionic conductivity in LaH$_{3-2x}$O$_x$ inferred from muon study

We performed muon spin rotation and relaxation ($\mu$SR) experiments to investigate the microscopic mechanism behind the high ionic conductivity ($\sigma$) exhibited by hydride (H$^-$) ions in lanthanum hydroxide LaH$_{3-2x}$O$_x$. The $\mu$SR spectra observed at 5--300 K in a sample with $x\approx0.25$ consist primarily of two components which are attributed to muons occupying tetrahedral (Tet) and octahedral (Oct) sites common to H$^-$. The spectra also indicate that muons at the Oct sites (Mu$_{\rm O}$) appear nearly stationary in the time scale of $\mu$SR ($\sim$10$^{-5}$ s), whereas those at the Tet sites (Mu$_{\rm T}$) are subject to the fluctuating local fields. The cusp-like peak in the fluctuation rate around 160 K and the decrease in linewidth at higher temperatures probed by Mu$_{\rm T}$ suggest that the jump motion of both Mu$_{\rm T}$ (via the vacant Oct sites) and surrounding Oct-site H$^-$ contributes to spin relaxation and that the fluctuation frequency is widely distributed. These results indicate that the implanted Mu behave as Mu$^-$ and that the jump motion of Mu$^-$/H$^-$ is restricted by the availability of nearby vacant sites. On the other hand, the activation energy for the jump is estimated to be 0.11(3) eV, which is significantly different from $\sim$1.3 eV evaluated from the temperature dependence of $\sigma$ at high temperatures ($\gtrsim400$ K). In our attempt to resolve this discrepancy, we discuss problems inherent in interpreting $\sigma$ using the Arrhenius equation, and demonstrate that the behavior of H$^-$ ions can be better explained as a viscous fluid exhibiting a glass transition.

cond-mat.mtrl-sci↗

arXiv2025

Cu-spin Correlation in the Electron-overdoped High-Tc Cuprate Thin Films of La_2-x_Ce_x_CuO_4_ Probed by Low-energy Muons

We investigated the Cu-spin correlation in the overdoped regime of the electron-doped high-Tc cuprate thin films of La_2-x_Ce_x_CuO_4_, changing the reduction condition from muon spin relaxation using low-energy muons. The Cu-spin correlation developed at low temperatures for optimally reduced films with x=0.13 as well as x=0.17 where the superconductivity was almost suppressed. These results are contrary to those observed in the hole-doped high-Tc cuprates where the development of the antiferromagnetic Cu-spin correlation disappears together with the suppression of superconductivity. The Cu-spin correlation developed at low temperatures in x=0.17 may be understood in terms of antiferromagnetism, but it may be related to a ferromagnetic order recently suggested in the nonsuperconducting heavily overdoped La$_2-x_Ce_x_CuO_4_ with x~0.18.

cond-mat.supr-con↗

arXiv2025

Molecular dynamics of $cis$-polybutadiene across the glass transition revealed by muonated-radical spin relaxation

The local molecular motion of $cis$-polybutadiene, a typical polymeric material exhibiting a glass transition ($T_{\rm g}=168$ K), is investigated by the spin relaxation of muonated radicals, where the relaxation is induced by the fluctuation of hyperfine (HF) fields exerted from an unpaired electron to a nearby muon and surrounding protons. The relaxation rate $1/T_\mu$ measured under various longitudinal magnetic fields is analyzed using the recently developed theory of spin relaxation to consider the coexistence of quasistatic and fluctuating HF fields, where the fluctuation frequency for the latter $\nu$ is evaluated over a temperature $T$ range of 5-320 K. The obtained $\nu(T)$ is found to be well reproduced by the Arrhenius relation, and the activation energy and preexponential factor are in good agreement with those for the "elemental process" revealed by quasielastic neutron scattering and attributed to a fluctuation across three carbon-carbon bonds. This result demonstrates that muonated-radical spin relaxation is a promising approach for direct access to local molecular motions in the sub-nanosecond range and for their detailed modeling at the atomic scale.

cond-mat.mtrl-sci↗

arXiv2025

Correlation between ferroelectricity and torsional motion of acetyl groups in tris(4-acetylphenyl)amine observed by muon spin relaxation

It is demonstrated by muon spin relaxation and resonance experiments that the switchable spontaneous polarization of the organic ferroelectric compound tris(4-acetylphenyl)amine (TAPA) is governed by the local molecular dynamics of the acetyl group. The implanted muon forms paramagnetic states which exhibit longitudinal spin relaxation due to the fluctuation of hyperfine fields exerted from unpaired electrons. The first-principle density functional theory calculations indicate that these states are muonated radicals localized at the phenyl group and on the carbon/oxygen of the acetyl group, thereby suggesting that the spin relaxation is dominated by the random torsional motion of acetyl group around the CC bond to the phenyl group. The stepwise change in the relative yield of radicals at $T_0\approx 350$ K and the gradual increase in the spin relaxation rate with temperature ($T$) indicate that the torsional motion is significantly enhanced by thermal excitation above $T_0$. This occurs concomitantly with the strong enhancement in the atomic displacement parameter of oxygen in the acetyl group (which is non-linear in $T$), indicating that it is the local molecular motion of the acetyl groups that drives the structural transition.

cond-mat.mtrl-sci↗

arXiv2024

Improved measurements of neutron lifetime with cold neutron beam at J-PARC

The ``neutron lifetime puzzle'' arises from the discrepancy between neutron lifetime measurements obtained using the beam method, which measures decay products, and the bottle method, which measures the disappearance of neutrons. To resolve this puzzle, we conducted an experiment using a pulsed cold neutron beam at J-PARC. In this experiment, the neutron lifetime is determined from the ratio of neutron decay counts to $^3$He(n,p)$^3$H reactions in a gas detector. This experiment belongs to the beam method but differs from previous experiments that measured protons, as it instead detects electrons, enabling measurements with distinct systematic uncertainties. By enlarging the beam transport system and reducing systematic uncertainties, we achieved a fivefold improvement in precision. Analysis of all acquired data yielded a neutron lifetime of $\tau_{\rm n}=877.2~\pm~1.7_{\rm(stat.)}~^{+4.0}_{-3.6}{}_{\rm (sys.)}$ s. This result is consistent with bottle method measurements but exhibits a 2.3$\sigma$ tension with the average value obtained from the proton-detection-based beam method.

nucl-ex↗

arXiv2024

Field-Induced Criticality in YbCu4Au

YbCu4Au is a unique material exhibiting multiple quantum fluctuations simultaneously. In this study, we investigated the field-induced criticality in YbCu4Au, based on comprehensive micro and macro measurements, including powder X-ray diffraction (XRD), neutron powder diffraction (NPD), nuclear magnetic resonance, magnetization, resistivity, specific heat, muon spin rotation relaxation (muSR), and X-ray absorption spectroscopy (XAS). Single crystals of YbCu4Au were grown, and their crystal structure was determined using XRD, and NPD measurements. Magnetic successive transitions were observed below 1 T by specific heat, resistivity, NPD, and muSR measurements. XAS measurements further indicate that the valence of Yb ions (+2.93) remained unchanged above 2 T. Moreover, the change in quadrupole frequency observed in the previous study is attributable to the electric quadrupole, as the expected value of the electric quadrupole was finite under magnetic fields [S. Wada et al., Journal of Physics: Condensed Matter, 20, 175201 (2008).]. These experimental results suggest that YbCu4Au exhibited bicritical behavior near 1 T, arising from the competition between RKKY interaction, accounting for the magnetic phases, and the Zeeman effect.

cond-mat.str-el↗

arXiv2024

Spontaneous magnetic field and disorder effects in BaPtAs_1-x_Sb_x_ with honeycomb network

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 (muSR) results of layered pnictide BaPtAs_1-x_Sb_x_ with a honeycomb network composed of Pt and (As, Sb). We observed an increase of the zero-field muon-spin relaxation rate in the superconducting (SC) state at the Sb end of x=1.0, suggesting the occurrence of spontaneous magnetic field due to the time-reversal symmetry breaking in the SC state. On the other hand, spontaneous magnetic field was almost and completely suppressed for the As-Sb mixed samples of x=0.9 and 0.2, respectively, suggesting that the time-reversal symmetry breaking SC state in x=1.0 is sensitive to disorder. The magnetic penetration depth estimated from transverse-field muSR measurements at x=1.0 and 0.2 behaved like weak-coupling s-wave superconductivity. These seemingly incompatible zero-field and transverse-field muSR results of BaPtAs_1-x_Sb_x_ with x=1.0 could be understood in terms of chiral d-wave superconductivity with point nodes on the three-dimensional Fermi surface.

cond-mat.supr-con↗

arXiv2024

Slow polymer dynamics in poly(3-hexylthiophene) probed by muon spin relaxation

The molecular dynamics of regioregulated poly(3-hexylthiophene) P3HT is investigated using muon spin relaxation ($\mu$SR). The response of the $\mu$SR spectra to a longitudinal magnetic field ($B_{\rm LF}$, parallel to the initial muon spin direction) indicates that the implanted muons form both muonated radicals localized on the thiophene ring and diamagnetic states with comparable yields. Moreover, the unpaired electron in the radical undergoes hyperfine interactions with muon bound to thiophene and with neighboring protons, whose fluctuations can serve as a measure for the molecular dynamics. The $B_{\rm LF}$ dependence of the longitudinal muon spin relaxation rate ($1/T_{1\mu}$) measured in detail at several temperatures is found to be well reproduced by the spectral density function $J(\omega)$ derived from the local susceptibility that incorporates the Havriliak-Negami (H-N) function used in the analysis of dielectric relaxation, $\chi(\omega)\propto1/[1-i(\omega/\tilde{\nu})^\delta]^\gamma$ (where $\tilde{\nu}$ is the mean fluctuation rate, and $0<\gamma, \delta\le1$). The magnitude of $\tilde{\nu}$ and its temperature dependence deduced from the analysis of $1/T_{1\mu}$ are found to be consistent with the motion of hexyl chains and thiophene rings suggested by $^{13}$C-NMR. The present result marks a methodological milestone in the application of $\mu$SR to the dynamics of complex systems with coexisting fluctuations over a wide range of time scales, such as polymers.

cond-mat.mtrl-sci↗

arXiv2024

Nonmagnetic Ground State in RuO$_2$ Revealed by Muon Spin Rotation

The magnetic ground state of single crystalline RuO$_2$ was investigated by the muon spin rotation/relaxation ($\mu$SR) experiment. The spin precession signal due to the spontaneous internal magnetic field $B_{\rm loc}$, which is expected in the magnetically ordered phase, was not observed in the temperature range 5--400~K. Muon sites were evaluated by first-principles calculations using dilute hydrogen simulating muon as pseudo-hydrogen, and $B_{\rm loc}$ was simulated for the antiferromagnetic (AFM) structures with a Ru magnetic moment $|{\bf m}_{\rm Ru}|\approx0.05\mu_\mathrm{B}$ suggested from diffraction experiments. As a result, the possibility was ruled out that muons are localized at sites where $B_{\rm loc}$ accidentally cancels. Conversely, assuming that the slow relaxation observed in $\mu$SR spectra was part of the precession signal, the upper limit for the magnitude of $|{\bf m}_{\rm Ru}|$ was estimated to be $4.8(2)\times10^{-4}\mu_{\rm B}$, which is significantly less than $0.05\mu_\mathrm{B}$. These results indicate that the AFM order, as reported, is unlikely to exist in the bulk crystal.

cond-mat.str-el↗

arXiv2024

Nano-scale dynamics of hydrogen in VO$_{2}$ studied by $\mu $SR

Hydrogen dynamics in the nanoscale region of VO$_{2}$ was investigated by muon spin rotation/relaxation ($\mu $SR) technique. Positively charged muon acts as a light radioisotope of proton and can be used as a probe to explore the inside of materials from an atomic perspective. By analyzing the muon hopping rate and the spatial distribution of the $^{51}$V nuclear magnetic moments, we have identified two types of diffusion paths in VO$_{2}$ (via oxygen-muon bonds or defects) and the potential of a high diffusion coefficient in the 10$^{-10}$ cm$^{2}$/s range at ambient temperature. Our results provide valuable information for developing hydrogen-driven VO$_{2}$--related electronic devices.

cond-mat.mtrl-sci↗

arXiv2024

Local electronic structure of dilute hydrogen in $\beta$-MnO$_{2}$

The electronic and magnetic states of $\beta$-MnO$_{2}$ in terms of hydrogen impurities have been investigated by muon spin rotation ($\mu$SR) technique combined with density-functional theory (DFT) calculations for muon as pseudo-hydrogen. We found that 85% of implanted muons are localized in the oxygen channels of the rutile structure and behave as interstitial protons (Mu$^{+})$ except those (7.6%) forming a charge-neutral state (Mu$^{0})$ at 2.3 K, which indicates that interstitial hydrogen acts as a shallow donor within less than 0.1 meV of ionization energy. The residual 15% of muons are attributed to those related to lattice imperfection as Mn vacancies. Detailed analyses combined with DFT approach suggested that the muon is localized at the center of the oxygen channel due to its large zero-point vibration energy.

cond-mat.mtrl-sci↗

arXiv2023

Performance of the Fully-equipped Spin Flip Chopper For Neutron Lifetime Experiment at J-PARC

To solve the ''neutron lifetime puzzle,'' where measured neutron lifetimes differ depending on the measurement methods, an experiment with pulsed neutron beam at J-PARC is in progress. In this experiment, neutrons are bunched into 40-cm lengths using a spin flip chopper (SFC), where the statistical sensitivity was limited by the aperture size of the SFC. The SFC comprises three sets of magnetic supermirrors and two resonant spin flippers. In this paper, we discuss an upgrade to enlarge the apertures of the SFC. With this upgrade, the statistics per unit time of the neutron lifetime experiment increased by a factor of 2.8, while maintaining a signal-to-noise ratio of 250-400 comparable to the previous one. Consequently, the time required to reach a precision of 1 s in the neutron lifetime experiment was reduced from 590 to 170 days, which is a significant reduction in time. This improvement in statistic will also contribute to the reduction of systematic uncertainties, such as background evaluation, fostering further advancements in the neutron lifetime experiments at J-PARC.

physics.ins-det↗

arXiv2023

Development of Transient $\mu$SR Method for High-Flux Pulsed Muons

In order to expand the applicability of muon spin rotation, relaxation, and resonance ($\mu$SR) experiments with pulsed muons and to make effective use of the high-flux beam, we have developed a new experimental method ``transient $\mu$SR''. In this method, $\mu$SR data for each muon pulse are tagged with external parameters such as temperature and magnetic field in real time, allowing the sample environment to be changed without interrupting data collection. As a result, continuous $\mu$SR measurements under sample conditions that vary on a time scale longer than the beam pulse interval (40 ms) are realized, and efficient beam utilization is achieved by eliminating the lag time associated with moving between discrete measurement points. The transient $\mu$SR method was applied to the study of the magnetic properties of cupric oxide (CuO) and the observation of level-crossing resonance relaxation in copper, and the method was successfully established by confirming that the results reproduce those in the previous reports.

physics.ins-det↗

arXiv2023

Photo-excited charge carrier lifetime enhanced by slow cation molecular dynamics in lead iodide perovskite FAPbI$_3$

Using muon spin relaxation ($\mu$SR) measurements on formamidinium lead iodide [FAPbI$_3$, where FA denotes HC(NH$_2)_2$] we show that, among the five structurally distinct phases of FAPbI$_3$ exhibited through two different temperature hysteresis, the reorientation motion of FA molecules is quasi-static below $\approx50$ K over the time scale of 10$^{-6}$ s in the low-temperature (LT) hexagonal (Hex-LT, $<160$ K) phase which has relatively longer photo-excited charge carrier lifetime ($\tau_{\rm c}\sim$10$^{-6}$ s). In contrast, a sharp increase in the FA molecular motion was found above $\approx50$ K in the Hex-LT phase, LT-tetragonal phase (Tet-LT, $<140$ K), the high-temperature (HT) hexagonal phase (Hex-HT, 160-380 K), and the HT-tetragonal phase (Tet-HT, 140-280 K) where $\tau_{\rm c}$ decreases with increasing temperature. More interestingly, the reorientation motion is further promoted in the cubic phase at higher temperatures ($>380/280$ K), while $\tau_{\rm c}$ is recovered to comparable or larger than that of the LT phases. These results indicate that there are two factors that determine $\tau_{\rm c}$, one related to the local reorientation of cationic molecules that is not unencumbered by phonons, and the other to the high symmetry of the bulk crystal structure.

cond-mat.mtrl-sci↗

arXiv2023

Direct observation of oxygen polarization in Sr$_2$IrO$_4$ by O $K$-edge x-ray magnetic circular dichroism

X-ray absorption spectroscopy (XAS) and magnetic circular dichroism (XMCD) measurements at the oxygen (O) $K$-edge were performed to investigate the magnetic polarization of ligand O atoms in the weak ferromagnetic (WFM) phase of the Ir perovskite compound Sr$_2$IrO$_4$. With the onset of the WFM phase below $T_{\rm N}\simeq240$ K, XMCD signals corresponding to XAS peaks respectively identified as originating from the magnetic moments of apical and planar oxygen (O$_{\rm A}$ and O$_{\rm P}$) in the IrO$_6$ octahedra were observed. The observation of magnetic moments at O$_{\rm A}$ sites is consistent (except for the relative orientation) with that suggested by prior muon spin rotation ($\mu$SR) experiment in the non-collinear antiferromagnetic (NC-AFM) phase below $T_{\rm M}\approx100$ K. Assuming that the O$_{\rm A}$ magnetic moment observed by $\mu$SR is also responsible for the corresponding XMCD signal, the magnetic moment of O$_{\rm P}$ is estimated to be consistent with the previous $\mu$SR result. Since the O$_{\rm A}$ XMCD signal is mainly contributed by Ir 5$d$ $zx$ and $yz$ orbitals which also hybridize with O$_{\rm P}$, it is inferred that the relatively large O$_{\rm P}$ magnetic moment is induced by Ir 5$d$ $xy$ orbitals. Moreover, the inversion of O$_{\rm A}$ moments relative to Ir moments between the two magnetic phases revealed by XMCD suggests the presence of competing magnetic interactions for O$_{\rm A}$, with which the ordering of O$_{\rm A}$ moments in the NC-AFM phase may be suppressed to $T_{\rm M}$.

cond-mat.str-el↗

arXiv2023

Local electronic structure of dilute hydrogen in $\beta$-Ga$_2$O$_3$ probed by muons

The local electronic structure of muons (Mu) as dilute pseudo-hydrogen in single-crystalline $\beta$-Ga$_2$O$_3$ has been studied by the muon spin rotation/relaxation ($\mu$SR). High-precision measurements over a long time range of $\sim$25 $\mu$s have clearly identified two distinct Mu states: a quasi-static Mu (Mu$_1$) and fast-moving Mu (Mu$_2$). By comparing this result with predictions from the recently established ambipolarity model, these two states are respectively attributed to the relaxed-excited states associated with the donor ($E^{+/0}$) and acceptor ($E^{-/0}$) levels predicted by density functional theory (DFT) calculations for the interstitial H. Furthermore, the local electronic structure of Mu$_1$ is found to be an OMu-bonded state with three-coordinated oxygen. The structure is almost identical with the thermal equilibrium state of H, and it is found to function as an electron donor. The other Mu$_2$ is considered to be in the hydride state (Mu$^-$) from the ambipolarity model, suggesting that it is in fast diffusion motion through the short-lived neutral state due to the charge exchange reaction with conduction electrons (Mu$^0+e^-\rightleftarrows$Mu$^-$).

cond-mat.mtrl-sci↗

arXiv2022

Local electronic structure of interstitial hydrogen in MgH$_2$ inferred from muon study

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 $^\circ$C required for decomposition are major obstacles to small-scale applications such as automobiles. The local electronic structure of interstitial H in MgH$_2$ 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$_2$ 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, stabilizes the interstitial H$^-$ state.

cond-mat.mtrl-sci↗