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The molecular triangular lattice system, beta'-EtMe3Sb[Pd(dmit)2]2, is considered as a candidate material for the quantum spin liquid (QSL) state, although ongoing debates arise from recent controversial results. Here, the results of electron spin resonance (ESR) and muon spin relaxation (muSR) measurements on beta'-EtMe3Sb[Pd(dmit)2]2 are presented. Both results indicate characteristic behaviors related to quasi-one-dimensional (q1D) spin dynamics, whereas the direction of anisotropy found in ESR is in contradiction with previous theories. We succeed in interpreting the experiments by combining density-functional theory calculations and analysis of the effective model taking into account the multi-orbital nature of the system. While the QSL-like origin of beta'-EtMe3Sb[Pd(dmit)2]2 was initially attributed to the magnetic frustration of the triangular lattice, it appears that the primary origin is a 1D spin liquid resulting from the dimensional reduction effect., Comment: 5 pages, 4 figures

Existence of 1D spin diffusion in the electrochemical sugar recognition system consisting of a nano-sized gold particle (GNP), a ruthenium complex and a phenylboronic acid was investigated by NMR and muSR. When sugar molecules are recognized by the phenylboronic site, the response of electrochemical voltammetry of the Ru site changes, enabling the system to work as a sensitive sugar-sensor. In this recognition process, the change in the electronic state at the boron site caused by sugar must be transferred to the Ru site via alkyl chains. We have utilized the muon-labelled electrons method and the proton NMR to find out a channel of the electron transfer from the phenylboronic acid site to the gold nano particle via the one dimensional alkyl chain. If this transfer is driven by diffusive spin channel, characteristic field dependence is expected in the longitudinal spin relaxation rate of muSR and 1H-NMR. We have observed significant decrease in the spin relaxation rates with increasing applied field. The result is discussed in terms of low dimensional spin diffusion.

We report on the quantum criticality of YbCu$_4$Ni as revealed by our combined micro- and macro-measurements. We determine the crystal structure of YbCu$_4$Ni with site mixing by neutron diffraction measurements, which suggests the possible presence of Kondo disorder. However, decreasing the local spin susceptibility distribution and the development of spin fluctuations below 10 K at ambient pressure by muon spin rotation and relaxation measurements suggests that YbCu4Ni exhibits quantum criticality. Therefore, our experimental results indicate that YbCu4Ni is a new material that exhibits quantum criticality under a zero magnetic field and ambient pressure., Comment: 8 pages, 5 figures

In this work we present systematic set of measurements carried out by muon spin rotation/relaxation ($\mu^+$SR) and neutron powder diffraction (NPD) on the solid solution Na$_{\rm x}$Ca$_{1- \rm x}$Cr$_2$O$_4$. This study investigates Na-ion dynamics in the quasi-1D (Q1D) diffusion channels created by the honeycomb-like arrangement of CrO$_6$ octahedra, in the presence of defects introduced by Ca doping. With increasing Ca content, the size of the diffusion channels is enlarged, however, this effect does not enhance the Na ion mobility. Instead the overall diffusivity is hampered by the local defects and the Na hopping probability is lowered. The diffusion mechanism in Na$_{\rm x}$Ca$_{1- \rm x}$Cr$_2$O$_4$ was found to be interstitial and the activation energy as well as diffusion coefficient were determined for all the members of the solid solution.

The on-site Coulomb potential, U, and the covalent state of electronic orbitals play key roles for the Cooper pair symmetry and exotic electromagnetic properties of high-Tc superconducting cuprates. In this paper, we demonstrate a way to determine the value of U and present the whole picture of the covalent state of Cu spins in the mother system of the La-based high-Tc superconducting cuprate, La2CuO4, by combining the muon spin rotation ({\mu}SR) and the density functional theory (DFT) calculation. We reveal local deformations of the CuO6 octahedron followed by changes in Cu-spin distributions caused by the injected muon. Adjusting the DFT and muSR results, U and the minimum charge-transfer energy between the upper Hubbard band and the O 2p band were optimized to be 4.87(4) and 1.24(1) eV, respectively., Comment: 11 pages, 10 figures see https://link.aps.org/doi/10.1103/PhysRevResearch.4.033044

The muon spin relaxation method ({\mu}SR) is a powerful microscopic tool to probe electronic states of materials observing local magnetic field distributions on the muon. It often happens that a distribution of local magnetic fields shows intermediate state between Gaussian and Lorentzian shapes. In order to generally describe intermediate field distributions, we dealt the convolution of two isotropic distributions in the three dimension and derived exact muon-spin relaxation functions which can be applied to all crossover regimes between the Gaussian and Lorentzian., Comment: 23 pages, 10 figures, see https://doi.org/10.1093/ptep/ptab074

We have investigated the low-temperature magnetism of sodium superoxide (NaO$_{2}$), in which spin, orbital, and lattice degrees of freedom are closely entangled. The magnetic susceptibility shows anomalies at $T_{1}=220$ K and $T_{2}=190$ K, which correspond well to the structural phase transition temperatures, and a sudden decrease below $T_{3}=34$ K. At 4.2 K, the magnetization shows a clear stepwise anomaly around 30 T with a large hysteresis. In addition, the muon spin relaxation experiments indicate no magnetic phase transition down to $T=0.3$ K. The inelastic neutron scattering spectrum exhibits magnetic excitation with a finite energy gap. These results confirm that the ground state of NaO$_{2}$ is a spin-singlet state. To understand this ground state in NaO$_{2}$, we performed Raman scattering experiments. All the Raman-active libration modes expected for the marcasite phase below $T_{2}$ are observed. Furthermore, we find that several new peaks appear below $T_{3}$. This directly evidences the low crystal symmetry, namely, the presence of the phase transition at $T_{3}$. We conclude the singlet-ground state of NaO$_{2}$ due to the spin-Peierls instability., Comment: 6 pages, 3 figures

Despite its unique structural features, the magnetism of single-layered cuprate with five oxygen coordination ($T$*-type structure) has not been investigated thus far. Here, we report the results of muon spin relaxation and magnetic susceptibility measurements to elucidate the magnetism of $T$*-type La$_{1-x/2}$Eu$_{1-x/2}$Sr$_x$CuO$_4$ (LESCO) via magnetic Fe- and non-magnetic Zn-substitution. We clarified the inducement of the spin-glass (SG)-like magnetically ordered state in La$_{1-x/2}$Eu$_{1-x/2}$Sr$_x$Cu$_y$Fe$_{1-y}$O$_4$ with $x = 0.24 + y$, and the non-magnetic state in La$_{1-x/2}$Eu$_{1-x/2}$Sr$_x$Cu$_y$Zn$_{1-y}$O$_4$ with $x$ = 0.24 after the suppression of superconductivity for $y$ $\geq$ 0.025. The SG state lies below $\sim$7 K in a wide Sr concentration range between 0.19 and 0.34 in 5$\%$ Fe-substituted LESCO. The short-range SG state is consistent with that originating from the Ruderman-Kittel-Kasuya-Yosida interaction in a metallic state. Thus, the results provide the first evidence for Fermi liquid (FL) state in the pristine $T$*-type LESCO. Taking into account the results of an oxygen $K$-edge X-ray absorption spectroscopy measurement $[$J. Phys. Soc. Jpn. 89, 075002 (2020)$]$ reporting the actual hole concentrations in LESCO, our results demonstrate the existence of the FL state in a lower hole-concentration region, compared to that in $T$-type La$_{2-x}$Sr$_x$CuO$_4$. The emergence of the FL state in a lower hole-concentration region is possibly associated with a smaller charge transfer gap energy in the parent material with five oxygen coordination., Comment: 8 pages, 6 figures, accepted for publication in Phys. Rev. B

We investigated the magnetism and superconductivity in as-sintered (AS) and oxidation annealed (OA) T*-type La$_{1-x/2}$Eu$_{1-x/2}$Sr$_x$CuO$_4$ (LESCO) with 0.14 $\leq x \leq$ 0.28 by the first comprehensive muon spin rotation/relaxation ($\mu$SR), magnetic susceptibility, and electrical resistivity measurements. In OA superconducting samples, no evidence of magnetic order was observed, whereas AS semiconducting samples exhibited evidence of a disordered magnetic state in the measured temperature range between $\sim$4 K and $\sim$8 K. Therefore, the ground state in LESCO drastically varies with oxidation annealing and the magnetic phase competitively exists with the superconducting (SC) phase. The magnetic phase in the AS LESCO is quite robust against Sr doping, while the SC phase degrades with increasing $x$. A monotonous decrease of the SC transition temperature from 24.5 K in $x$ = 0.14 to 9.0 K in $x$ = 0.28 suggests the disappearance of the SC phase at $x$ $\sim$ 0.34. Furthermore, we clarified the simultaneous development of (quasi) static magnetism and the electrical resistivity at a low temperature in AS samples, suggesting the inducement of magnetism by the suppression of carrier mobility. The variation in magnetism due to annealing is discussed from a viewpoint of structural defects, which was previously reported from neutron diffraction measurements.

We demonstrate the presence of ferromagnetic (FM) fluctuations in the superconducting and non-superconducting heavily overdoped regimes of high-temperature superconducting copper oxides, using (Bi,Pb)_2_Sr_2_CuO_6+delta_ (Bi-2201) single crystals. Magnetization curves exhibit a tendency to be saturated in high magnetic fields at low temperatures in the heavily overdoped crystals, which is probably a precursor phenomenon of a FM transition at a lower temperature. Muon spin relaxation detects the enhancement of spin fluctuations at high temperatures below 200 K. Correspondingly, the ab-plane resistivity follows a 4/3 power law in a wide temperature range, which is characteristic of metals with two-dimensional FM fluctuations due to itinerant electrons. As the Wilson ratio evidences the enhancement of spin fluctuations with hole doping in the heavily overdoped regime, it is concluded that two-dimensional FM fluctuations reside in the heavily overdoped Bi-2201 cuprates, which is probably related to the decrease in the superconducting transition temperature in the heavily overdoped cuprates., Comment: 6 pages, 4 figures

Alkali superoxide CsO2 is one of candidates for the spin-1/2 one-dimensional (1D) antiferromagnet, which may be sequentially caused by an ordering of the pi-orbital of O2- molecule below TS ~ 70 K. Here, we report on the magnetism in powder CsO2 and high-magnetic field magnetization measurements in pulsed-magnetic fields of up to 60 T. We obtained the low temperature phase diagram around the antiferromagnetic ordering temperature TN = 9.6 K under the magnetic field. At 1.3 K, remarkable up-turn curvature in the magnetization around a saturation field of ~ 60 T is found, which corresponds to the spin-1/2. We will compare it with the theoretical calculation., Comment: 11 pages, 3 figures

Magnetic properties of a one-dimensional frustrated quantum spin system Rb2Cu2Mo3O12 is investigated by the muon spin relaxation (muSR) technique. Although this system shows an incommensurate spin correlation in neutron scattering, it has not yet been determined whether the ground state reaches to a nonmagnetic spin-singlet state or not. In this study, our zero-field (ZF) muSR result undoubtedly reveals a nonmagnetic ground state, which establishes formation of the nonmagnetic incommensurate spin-singlet state in combination of the previous neutron scattering study. Furthermore, we found that the internal field is slightly enhanced below ~7 K. This temperature dependence resembles that of electric polarization under the magnetic field reported recently, indicating a possibility that a small change occurs even under ZF. In longitudinal-field measurements, a fast fluctuation around a narrowing region is observed. This relaxation is expected to reflect characteristics of formation of the spin-singlet state., Comment: 5 pages, 3 figures, to be published in J. Phys. Soc. Jpn.: Conf. Proc

To clarify the magnetic properties of cluster-glass states in Sr1-xLaxRuO3 (0.3 <= x <= 0.5), we report herein the results of muon spin relaxation (muSR) and neutron powder diffraction measurements. The muSR experiments showed that magnetic clusters start developing well above the peak temperature T^* in the ac susceptibility. The volume fraction of the magnetically ordered region increases continuously with decreasing temperature, showing no anomaly at T^*, and reaches nearly 100% at the lowest temperature. The temperature variation of the volume fraction is essentially independent of the La concentration in the x range presently investigated, although the dc magnetization is significantly suppressed with increasing x. Neutron powder diffraction experiments revealed that the ground state for x = 0.3 is a long-range ferromagnetic ordered state. These results indicate that, with decreasing temperature, cluster-glass states in Sr1-xLaxRuO3 gradually develop into long-range ferromagnetic ordered states with decreasing temperature, and that the magnetic ordering process differs strikingly from that expected for a conventional second-order ferromagnetic transition., Comment: 8 pages, 8 figures, to appear in J. Phys. Soc. Jpn

In order to investigate the relationship between the so-called stripe correlations and the high-Tc superconductivity, we have carried out magnetic susceptibility and zero-field muon-spin-relaxation measurements in partially Fe-substituted La2-xSrxCu1-yFeyO4 (LSCFO). It has been found that the Fe substitution induces successive magnetic transitions in the overdoped regime, namely, a spin-glass transition of Fe3+ spins due to the RKKY interaction based on itinerant spins at higher temperatures and a stripe-order transition of localized Cu2+ spins at lower temperatures. The stripe-order transition disappears at the hole concentration of ~0.28 per Cu which coincides with the endpoint of the superconductivity in pristine La2-xSrxCuO4, suggesting that the stripe correlations are closely related to the high-Tc superconductivity in the overdoped regime as well as in the underdoped regime. As for the spin-glass state, it has been found that the contribution of polarized itinerant spins to the muon-spin depolarization is not negligible. Taking into account neutron-scattering results by R.-H. He et al. [Phys. Rev. Lett. 107, 127002 (2011)] that a spin-density-wave (SDW) order has been observed in overdoped LSCFO, the present results demonstrate the presence of a novel coexistent state of a SDW order and a spin-glass state., Comment: 8 pages, 5 figures

Muon spin relaxation on Nd$_2$Ti$_2$O$_7$ (NTO) and NdLaTi$_2$O$_7$ (NLTO) compounds are presented. The time spectra for both compounds are as expected for the paramagnetic state at high temperatures, but deviate from the exponential function below about 100 K. The muon spin relaxation rate increases with decreasing temperature firstly, and then levels off below about 10 K, which is reminiscent of the frustrated systems. An enhancement of the relaxation rate by a longitudinal field in the paramagnetic state is observed for NTO, and eliminated by a magnetic dilution for the NLTO sample. This suggests that the spectral density is modified by a magnetic dilution and thus indicates that the spins behave cooperatively rather than individually. Zero-field measurement at 0.3 K indicates that the magnetic ground state for NTO is ferromagnetic.

We have used the pulsed muon source at ISIS to study high-temperature Na-ion dynamics in the quasi-one-dimensional (Q1D) metallic antiferromagnet NaV2O4. By performing systematic zero-field and longitudinal-field measurements as a function of temperature we clearly distinguish that the hopping rate increases exponentially above Tdiff=250 K. The data is well fitted to an Arrhenius type equation typical for a diffusion process, showing that the Na-ions starts to be mobile above Tdiff . Such results makes this compound very interesting for the tuning of Q1D magnetism using atomic-scale ion-texturing through the periodic potential from ordered Na-vacancies. Further, it also opens the door to possible use of NaV2O4 and related compounds in energy related applications., Comment: Accepted for publication in Journal of Physics: Conference Series (2014)

Longitudinal-field muon-spin-relaxation measurements have revealed inhomogeneous distribution of the internal magnetic field at temperatures above the bulk superconducting (SC) transition temperature, $T_{\rm c}$, in slightly overdoped Bi$_2$Sr$_2$Ca$_{1-x}$Y$_x$Cu$_2$O$_{8+\delta}$. The distribution width of the internal magnetic field, $\Delta$, evolves continuously with decreasing temperature toward $T_{\rm c}$. The origin of the increase in $\Delta$ is discussed in terms of the creation of SC domains in a sample., Comment: 14 pages, 4 figures, to appear in JPSJ

We present muon spin relaxation ($\mu$SR) and specific-heat versus temperature $C(T)$ measurements on polycrystalline and single-crystal samples of the pyrochlore magnet Yb$_2$Ti$_2$O$_7$. $C(T)$ exhibits a sharp peak at a $T_\mathrm{C}$ of 0.21 and 0.26~K for the single-crystal and polycrystalline samples respectively. For both samples, the magnetic entropy released between 50~mK and 30~K amounts to $R\ln2$ per Yb. At temperatures below $T_\mathrm{C}$ we observe a steep drop in the asymmetry of the zero-field $\mu$SR time spectra at short time scales, as well as a decoupling of the muon spins from the internal field in longitudinal magnetic fields of $\leq0.25$~T for both the polycrystalline and single-crystal samples. These muon data are indicative of static magnetic moments. Our results are consistent with the onset of long-range magnetic order in both forms of Yb$_2$Ti$_2$O$_7$., Comment: 6 pages, 4 figures, accepted to PRB