arXiv subjects

Yoshihiko Ihara

Publications and source records attributed to Yoshihiko Ihara.

At least 19 recordsLinked to original sources

arXiv2026

Magnetism and Electrical Conduction in Lightly-Doped Single-Layer High-$T_c$ Cuprate $\mathrm{La}_2\mathrm{CuO}_{4+δ}$

The temperature dependences of magnetization and electrical resistivity as well as their magnetic field dependences have been examined in lightly-doped single-layer cuprate $\mathrm{La}_2\mathrm{CuO}_{4+δ}$ (LCO, hole-doping level $p \, (2δ) \cong 0.03$) single crystals, in comparison with those in the extremely low doping region of $p \lesssim 0.015$ to uncover the intrinsic magnetism and electrical conduction of the $\mathrm{Cu\text{-}O}$ plane that exhibits both antiferromagnetic (AF) and superconducting (SC) orders simultaneously. In $p \cong 0.03$ SC LCO, the sub-lattice moments on $\mathrm{Cu}$ sites and their AF couplings are only $\sim 15\,\%$ smaller than those of the Mott-insulator parent material, suggesting that the localization of $\mathrm{Cu}$ $3d$ electrons remains very strong. Furthermore, we report that in the SC LCO, two-dimensional AF spin correlations develop rapidly from $T^* \cong 280\text{ K}$ towards Néel temperature $T_{\mathrm{N}} = 266\text{ K}$, where the out-of-plane resistivity starts to decrease largely. This might be responsible for the AF ordering at such a high temperature in the SC single-layer cuprate with $p \cong 0.03$.

cond-mat.supr-con↗

arXiv2026

Microscopic Magnetism of A(TiO)Cu4(PO4)4 (A = Ba, Pb, Sr): 31P and 63,65Cu NMR Study

We report a comprehensive NMR study of the chiral square-cupola antiferromagnet Pb(TiO)Cu$_4$(PO$_4$)$_4$ and compare its microscopic hyperfine and local-field parameters with the Ba/Sr analogues in the $A$(TiO)Cu$_4$(PO$_4$)$_4$ family. Above $T_{\rm N}\simeq 6.7$ K, the $^{31}$P Knight shift tracks the bulk susceptibility and yields nearly isotropic transferred hyperfine couplings $H_{\rm hf}^{[010]}=6.77(3)$ and $H_{\rm hf}^{[001]}=6.19(3)$ kOe/$μ_{\rm B}$. Below $T_{\rm N}$, the frequency-swept $^{31}$P spectrum splits into three lines, in contrast to the four-line pattern reported for BaTCPO. The line separation tracks the onset of the static $^{31}$P internal field with a power-law exponent $β\simeq 0.23$, consistent with quasi-two-dimensional criticality. Crystal-rotation $^{31}$P NMR in the ordered state resolves all eight symmetry-related P sites and their site-dependent anisotropy. In the ordered state, zero-field $^{63,65}$Cu NMR gives a Cu-site internal field $B_{\rm int}=14.50(6)$ T and a quadrupole frequency $ν_Q=32.72(5)$ MHz, while point-charge electric-field-gradient calculations including Sternheimer corrections yield an on-site Cu hole occupancy $n_d=0.20(4)$, consistent with a ligand-hole-dominated charge-transfer character. Comparing PbTCPO with BaTCPO and SrTCPO, we find that the transferred hyperfine coupling $H_{\rm hf}$ varies across the series, reflecting changes in local Cu-O-P covalency, whereas the ordered-state $^{31}$P internal field in PbTCPO is $69.5$ mT, considerably higher than in BaTCPO ($35.6$ mT) and SrTCPO ($34.6$ mT). This enhancement is not captured by dipolar terms alone and points to the combined effects of transferred contributions and stacking-dependent cancellation.

cond-mat.str-el↗

arXiv2026

NMR Determination of the Low-Field Magnetic Structure of the Cu-Based Mineral Rouaite Cu$_2$(OH)$_3$NO$_3$

Frustrated interactions in the Cu-based mineral rouaite with alternating antiferromagnetic and ferromagnetic spin chains, Cu$_2$(OH)$_3$NO$_3$, introduce non-trivial magnetic ground states and exotic excitations arising from them. We investigated the magnetic structure of Cu$_2$(OH)$_3$NO$_3$ by $^1$H- and $^2$H-NMR measurements on single crystals. The internal fields in the ordered state were microscopically measured using the H nuclear moments as a local probe. The directions of the ordered moments were determined by comparing the experimental results to model calculations. The obtained magnetic structure suggests the importance of Dzyaloshinskii-Moriya interactions in stabilizing the low-field magnetic structure. The present result advances the theoretical understanding of the low-field magnetic states and will enable exploration of the exotic magnetic states emerging in high magnetic fields.

cond-mat.str-el↗

arXiv2025

Boron Clusters for Metal-Free Water Splitting

Electron-deficient boron clusters are identified as a fundamentally new class of oxygen evolution reaction (OER) catalysts, entirely free of transition metals. Selective sodium extraction from NaAlB14 and Na2B29 via high-pressure diffusion control introduces hole doping into B12 icosahedral frameworks, resulting in OER activity exceeding that of Co3O4 by more than an order of magnitude, and exceptional durability under alkaline conditions. B12 clusters are known for their superchaotropic character, which destabilizes hydrogen bonding in water. In this system, H2O, instead of OH-, preferentially adsorbs on the catalyst surface, suggesting a distinct OER pathway mediated by molecular water. This adsorption behavior contrasts with conventional transition-metal oxides and reflects the unique interfacial properties of the boron clusters. Density functional theory reveals unoccupied p orbitals and unique local electric fields at the cluster surface, both of which could promote the water activation. These findings suggest a paradigm shift in OER catalysis, in which the unique interaction between B12 clusters and water drives the reaction, replacing the conventional role of redox-active metals. Hole-doped boron clusters thus offer a promising platform for designing high-performance and durable water-splitting catalysts, opening new avenues for OER design beyond conventional transition-metal chemistry.

cond-mat.mtrl-sci↗

arXiv2025

Superconductivity emerging from the N${é}$el state in ${\it infinite}$-${\it stage}$ single-layer cuprate La$_2$CuO$_{4+δ}$

In copper oxides (cuprates) with single CuO$_2$ layer such as La$_{2-x}$Ba(Sr)$_x$CuO$_4$, antiferromagnetism coexists with superconductivity at small doping levels $x$, where chemical disorders are significant. Here, we report that superconductivity occurs in a uniform and fully ordered N${é}$el state in a single-layer cuprate La$_2$CuO$_{4+δ}$ with a small amount of excess oxygen $(δ= 0.015)$ as demonstrated by the $^{139}$La nuclear quadrupole resonance measurement. A uniform oxygen distribution in the crystal is crucial for achieving microscopic phase coexistence and overcoming the miscibility gap associated with the staging instability; self-organized periodic oxygen arrangement driven by mobile oxygen atoms. This finding prompts the reconsideration of superconductivity in cuprates, highlighting that it can emerge in a robust N${é}$el state that retains sizable magnetic moments and hosts only a small carrier density.

cond-mat.supr-con↗

arXiv2025

Compositional Tuning in NaxAlB14 via Diffusion Control

A uniform Na distribution in NaxAlB14 was achieved using high-pressure diffusion control (HPDC), which promotes Na deintercalation through enhanced diffusion under high pressure, combined with post-annealing. NaxAlB14 with a non-stoichiometric Na composition is thermodynamically metastable, and conventional solid-state reactions with adjusted starting compositions typically result in the formation of stoichiometric NaAlB14 and side products. While HPDC alone typically leads to concentration gradients, intentionally halting the Na removal process before complete extraction, followed by annealing, enabled a uniform composition across the bulk. This allowed structural and electronic properties to be examined over a wide range of Na concentrations. As Na content decreased, electrical conductivity increased, and the optical band gap narrowed. NMR measurements showed an increase in the density of states at the Fermi level, consistent with DFT calculations predicting boron-related in-gap states. Boron vacancies at specific sites were found to generate deep levels near the band gap center, which can explain experimentally observed optical gap reduction. These results demonstrate that diffusion-controlling methods can be effectively applied to synthesize metastable compounds with tunable compositions in covalent frameworks. Furthermore, they provide a foundation for designing functional boride-based materials with adjustable electronic properties by controlling Na extraction and inducing defect formation.

cond-mat.mtrl-sci↗

arXiv2025

Magnetic excitations in the 1/3 plateau state in InCu$_3$(OH)$_6$Cl$_3$

Magnetic dynamics in InCu$_3$(OH)$_6$Cl$_3$ was investigated from the NMR relaxation rate measurement. In InCu$_3$(OH)$_6$Cl$_3$, the magnetization isotherm shows a plateau at the 1/3 of full-saturation magnetization, characterizing the 1/3 plateau state. As the 1/3 plateau state appears above 7 T upto 14 T, the microscopic magnetic properties were investigated with the NMR measurement in steady fields. The temperature and field dependence of $1/T_1$ measurement reveals a gap in the magnetic excitation spectrum and its evolution with field in the 1/3 plateau state. The field dependence of spin gap provides an important information to understand the microscopic origin of 1/3 plateau state in the kagome antiferromagnets.

cond-mat.str-el↗

arXiv2025

Probing Mixed Valence States by Nuclear Spin-Spin Relaxation Time Measurements

Several elements in the periodic table exhibit an interesting and often overlooked feature: They skip certain valence states which is discussed in the field of superconductivity to be in favor of fostering higher transition temperatures $T_c$. However, from the experimental point of view, it is often deemed difficult to probe changes in the valence state. Here we demonstrate that the latter are accessible by the spin-spin relaxation rate $1/T_2$ in nuclear magnetic resonance. As target material, we chose the solid solution Ge$_{1-x}$In$_x$Te, where valence-skipping In induces superconductivity and changes its valence state as a function of $x$. We observe a strong enhancement in $1/T_2(x)$ and, most importantly, find that $1/T_2$ and $T_c$ exhibit a strikingly similar $x$ dependence. These results underline the importance of valence physics for the evolution of superconductivity in Ge$_{1-x}$In$_x$Te. A model based on a Ruderman-Kittel-Kasuya-Yosida type of interaction among the In nuclei is proposed which fully accounts for the experimental results.

cond-mat.supr-con↗

arXiv2024

Nonlinear nonreciprocal electronic conductivity driven by magnetic field gradients

We theoretically propose the emergence of nonlinear nonreciprocal conductivity in centrosymmetric paramagnetic systems when a spatially gradient magnetic field is externally applied. The key essence lies in the appearance of magnetic toroidal dipole moment under the gradient field that breaks both spatial inversion and time-reversal symmetries. By analyzing a minimal tight-binding model on a two-dimensional system, we show that an effective coupling between the magnetic toroidal dipole moment arising from the gradient field and sublattice-dependent antisymmetric spin-orbit interaction plays an important role in inducing the nonlinear nonreciprocal transport. We also discuss the favorable situation to observe the nonlinear nonreciprocal conductivity in real materials by presenting an experimental setup in order to stimulate the findings.

cond-mat.str-el↗

arXiv2024

Magnetic Phase Diagram of Rouaite, Cu$_2$(OH)$_3$NO$_3$

Spinon-magnon mixing was recently reported in botallackite Cu$_2$(OH)$_3$Br with a uniaxially compressed triangular lattice of Cu$^{2+}$ quantum spins [Zhang et al., Phys. Rev. Lett. 125, 037204 (2020)]. Its nitrate counterpart rouaite, Cu$_2$(OH)$_3$NO$_3$, has a highly analogous structure and might be expected to exhibit similar physics. To lay a foundation for research on this material, we clarify rouaite's magnetic phase diagram and identify both low-field phases. The low-temperature magnetic state consists of alternating ferro- and antiferromagnetic chains, as in botallackite, but with additional canting, leading to net moments on all chains which rotate from one chain to another to form a 90$^\circ$ cycloidal pattern. The higher-temperature phase is a helical modulation of this order, wherein the spins rotate from one Cu plane to the next. This extends to zero temperature for fields perpendicular to the chains, leading to a set of low-temperature field-induced phase transitions. Rouaite may offer another platform for spinon-magnon mixing, while our results suggest a delicate balance of interactions and high tunability of the magnetism.

cond-mat.str-el↗

arXiv2022

Negative-chirality order in $S=1/2$ kagome antiferromagnet CdCu$_{3}$(OH)$_{6}$(NO$_{3}$)$_{2}\cdot $H$_{2}$O

The neutron diffraction and nuclear magnetic resonance (NMR) measurements have been used to microscopically analyze the magnetic structure in the $S = 1/2$ kagome antiferromagnet CdCu$_{3}$(OH)$_{6}$(NO$_{3}$)$_{2}\cdot $H$_{2}$O. Below the magnetic ordering temperature $T_N\simeq 4$ K, magnetic Bragg reflections at (110) and (100) were found in the neutron diffraction pattern, which suggests a $q=0$ magnetic structure. Furthermore, the vector spin chirality for the $q=0$ structure was successfully identified from the internal field direction obtained by the $^{14}$N-NMR measurement. Our findings point to a chirality-ordered magnetic structure with negative vector chirality and $\langle 100 \rangle$ anisotropy.

cond-mat.str-el↗

arXiv2021

NMR measurements in dynamically controlled field pulse

We present the architecture of the versatile NMR spectrometer with software-defined radio (SDR) technology and its application to the dynamically controlled pulsed magnetic fields. The pulse-field technology is the only solution to access magnetic fields greater than 50 T, but the NMR experiment in the pulsed magnetic field was difficult because of the continuously changing field strength. The dynamically controlled field pulse allows us to perform NMR experiment in a quasi-steady field condition by creating a constant magnetic field for a short time around the peak of the field pulse. We confirmed the reproducibility of the field pulses using the NMR spectroscopy as a high precision magnetometer. With the highly reproducible field strength we succeeded in measuring the nuclear spin-lattice relaxation rate $1/T_1$, which had never been measured by the pulse-field NMR experiment without dynamic field control. We also implement the NMR spectrum measurement with both the frequency-sweep and field-sweep modes and discuss the appropriate choice of these modes depending on the magnetic properties of sample to be measured. This development, with further improvement at a long-duration field pulse, will innovate the microscopic measurement in extremely high magnetic fields.

cond-mat.str-el↗

arXiv2021

Possible Magnetic Structure with a Tilted Helical Plane in SmBe13 Probed by 9Be-NMR Study

9Be-NMR measurements were performed using single crystalline SmBe13 in order to investigate a magnetic structure of a low-temperature ordering state microscopically. We observed a spectral broadening in the ordered state, and the broadened spectral shape depends on the magnetic field directions. By comparing the experimentally obtained and simulated NMR spectra for magnetic fields along the cubic [001] and [011] directions, we argue a helical structure with a basal plane tilted from the (001) plane in low-field ordering region under the assumption of a helical with a propagation vector of (0, 0, 1/3) found in other RBe13 compounds (R = rare earths). Such a tilted helical structure is explained by a combination of an ellipse helical in the (001) plane and a longitudinal magnetic density wave along the [001] direction. Considering a magnetic easy axis parallel to [001] revealed by the magnetization measurements, the peculiar helical structure in SmBe13 may be built on delicate balance among exchange interactions, dipole-dipole interaction, and single-ion magnetic anisotropy due to the crystalline electric field.

cond-mat.str-el↗

arXiv2021

Emergence of Frustrated Short-Range Order above Long-Range Order in the $S=1/2$ Kagome Antiferromagnet CaCu$_3$(OD)$_6$Cl$_2\cdot0.6$D$_2$O

We report on the low-energy dynamics in the kagome antiferromagnet CaCu$_3$(OD)$_6$Cl$_2\cdot0.6$D$_2$O (Ca-kapellasite) as studied by use of $^2$D-NMR measurements. Previous $^{35}$Cl-NMR measurements revealed that the nuclear spin-lattice relaxation rate ($1/T_1$) shows two peaks at temperatures, $T^{\ast} = 7.2$ K and $T_s \simeq 25$ K. While the low-temperature peak at $T^{\ast}$ is ascribed to the critical fluctuations near the long-range magnetic ordering, the origin of the high-temperature peak has not been fully understood. From the $1/T_1$ measurements on the D sites at the OD groups (D$_{\rm OD}$), we find no peak at $T_s$, evidencing that the high-temperature peak is not related to the molecular dynamics of the OD groups. We discuss the possibility of a frustration-induced short-range ordered state below $T_s$ before the long-range order is stabilized by the Dzyaloshinskii-Moriya interaction. We also observed static internal fields at the D$_{\rm OD}$ site in the long-range ordered state below $T^{\ast}$, and confirm the previously proposed negative-chirality $q=0$ magnetic structure.

cond-mat.str-el↗

arXiv2020

Symmetry lowering on the field-induced commensurate phase in CeRhIn$_5$

Temperature dependence of the $^{115}$In-NMR spectra of CeRhIn$_5$ is studied with the external magnetic fields 10$^\circ$ off the [100] and [001] axes. Our detailed analyses confirm that the AFM3 phase breaks the four-fold spin symmetry with the commensurate ordering vector of $Q = (0.5, 0.5,0.25)$. Based on the observation of anistropic hyperfine fields, we also propose the symmetry lowering of the electronic structure in the AFM3 phase.

cond-mat.str-el↗

arXiv2019

Microscopic coexistence of superconductivity and charge order in organic superconductor $β''$-(BEDT-TTF)$_{4}$[(H$_3$O)Ga(C$_2$O$_4$)$_3$]$\cdot$C$_6$H$_5$NO$_2$

The electron paramagnetic resonance study for an organic superconductor $β''$-(BEDT-TTF)$_{4}$[(H$_3$O)Ga(C$_2$O$_4$)$_3$]$\cdot$C$_6$H$_5$NO$_2$ reveals that superconductivity coexists uniformly with the charge ordered state in one material. In the charge ordered state, the interplane spin exchange is gapped, while the in-plane conductivity is not significantly modified. This anisotropic behavior is explained by the exotic charge ordered state, in which molecular-site selective carrier localization coexists with conducting carriers on other molecules. Relationship between superconductivity and this conductive charge ordered state is investigated.

cond-mat.supr-con↗

arXiv2013

NMR investigation of the pressure induced Mott transition to superconductivity in Cs3C60 isomeric compounds

The discovery in 1991 of high temperature superconductivity (SC) in A3C60 compounds, where A is an alkali ion, has been initially ascribed to a BCS mechanism, with a weak incidence of electron correlations. However various experimental evidences taken for compounds with distinct alkali content established the interplay of strong correlations and Jahn Teller distortions of the C60 ball. The importance of electronic correlations even in A3C60 has been highlighted by the recent discovery of two expanded fulleride Cs3C60 isomeric phases that are Mott insulators at ambient pressure. Both phases undergo a pressure induced first order Mott transition to SC with a (p, T) phase diagram displaying a dome shaped SC, a common situation encountered nowadays in correlated electron systems. NMR experiments allowed us to establish that the bipartite A15 phase displays Néel order at 47K, while magnetic freezing only occurs at lower temperature in the fcc phase. NMR data do permit us to conclude that well above the critical pressure, the singlet superconductivity found for light alkalis is recovered. However deviations from BCS expectations linked with electronic correlations are found near the Mott transition. So, although SC involves an electron-phonon mechanism, correlations have a significant incidence on the electronic properties, as had been anticipated from DMFT calculations.

cond-mat.str-el↗

arXiv2013

13C NMR study of superconductivity near charge instability realized in beta"-(BEDT-TTF)4[(H3O)Ga(C2O4)3]C6H5NO2

To investigate the superconducting (SC) state near a charge instability, we performed ^{13}C NMR experiments on the molecular superconductor beta"-(BEDT-TTF)_{4}[(H_{3}O)Ga(C_{2}O_{4})_{3}]C_{6}H_{5}NO_{2}, which exhibits a charge anomaly at 100 K. The Knight shift which we measured in the SC state down to 1.5 K demonstrates that Cooper pairs are in spin-singlet state. Measurements of the nuclear spin-lattice relaxation time reveal strong electron-electron correlations in the normal state. The resistivity increase observed below 10 K indicates that the enhanced fluctuation has an electric origin. We discuss the possibility of charge-fluctuation-induced superconductivity.

cond-mat.supr-con↗