arXiv subjects

Ryutaro Okuma

Publications and source records attributed to Ryutaro Okuma.

At least 19 recordsLinked to original sources

arXiv2026

Raman spectroscopy of van der Waals topological magnet GdGaI

We report polarization-resolved Raman spectroscopy of a van der Waals compound GdGaI that is a candidate for excitonic insulators. By combining the symmetry analysis with density functional theory calculations, we identify six Raman-active phonons. The spectra exhibit only the expected anharmonic hardening down to 4 K: no additional peaks, no soft modes, and no signatures of zone folding are observed. This result indicates that any lattice distortion is below our experimental sensitivity, supporting an electronically driven origin for the band reconstruction reported by angle-resolved photoemission spectroscopy rather than an electron-phonon-driven mechanism. Moreover, we observe a pronounced circular dichroism of the $A_{1g}$ modes under an out-of-plane magnetic field. Based on symmetry considerations, we attribute this dichroic response to chiral $A_{1g}$ phonons with opposite angular momenta generated by spin-phonon coupling in the time-reversal-broken state. The temperature evolution of the degree of circular polarization further suggests that circularly polarized Raman spectroscopy detects the emergence of short-range antiferromagnetic correlations. Our results highlight GdGaI as a promising platform in which excitonic order, magnetism, and circularly polarized phonons can be intertwined, and demonstrate that circular-polarization Raman provides a sensitive probe of spin-phonon coupling in excitonic systems.

cond-mat.mtrl-sci↗

arXiv2026

Stabilizing Itinerant Electrons in a Corner-Sharing Kagom\'e Oxide Nd4Os3ZnO14

Kagome oxides provide a fertile platform for exploring exotic electronic states arising from geometrical frustration and characteristic band topology. Here, we report the synthesis of a 5d transition-metal kagome oxide, Nd4Os3ZnO14, obtained via high-temperature, high-pressure hydrothermal synthesis. Single-crystal X-ray diffraction reveals a two-dimensional kagome network formed by corner-sharing OsO6 octahedra, with a nominal osmium valence of +4.67. In-plane resistivity and hard X-ray photoelectron spectroscopy measurements indicate that the semimetallic electronic structure at room temperature evolves into a semiconducting ground state upon cooling, accompanied by a pronounced enhancement of hole mobility. Magnetic susceptibility measurements demonstrate localized Nd3+ moments without long-range magnetic order down to 2 K. The coexistence of a metallic kagome plane, strong spin-orbit coupling inherent to 5d electrons, and rare-earth magnetism establishes Nd4Os3ZnO14 as a promising platform for investigating correlated electron phenomena in kagome oxides within the itinerant regime.

cond-mat.str-el↗

arXiv2026

Highly fluctuating double-$q$ magnetic order in the van der Waals metal CeTe$_3$

CeTe$_3$ is a van der Waals antiferromagnet composed of magnetic [CeTe]$^+$ layers coupled to highly conducting Te$^{0.5-}$ square nets. Its simple quasi-two-dimensional electronic structure and cleavable nature make it an appealing platform for exploring correlated magnetism in reduced dimensions. To clarify the nature of its low-temperature state, we performed single-crystal neutron diffraction down to 0.3 K, complemented by scanning tunneling microscopy. A magnetic transition near 1.5 K gives rise to incommensurate Bragg peaks at $q_{\pm}\sim(\pm0.17,0,0.31)$, consistent with a double-$q$ magnetic order whose moments are predominantly aligned along the $c$ axis. The strongly reduced ordered moment is consistent with enhanced quantum fluctuations driven by $c$-$f$ hybridization, while the deviation of the propagation vectors from simple nesting suggests a coupling to residual charge-density-wave instabilities of the quasi-one-dimensional Te-derived bands. These results indicate that CeTe$_3$ hosts a correlated magnetic ground state where spin and itinerant charge degrees of freedom are intimately linked in the van der Waals limit.

cond-mat.str-el↗

arXiv2026

Quasi-One-Dimensional Electronic Nature of Ta4SiTe4 Underlying the Giant Thermoelectric Performance

Ta4SiTe4 is a one-dimensional van der Waals material that exhibits an exceptionally large thermoelectric power factor below room temperature. However, since this material has been available only in the form of acicular microcrystals, experimental exploration of the electronic properties responsible for its giant thermoelectric performance has long been challenging. In this study, we quantitatively evaluated the one-dimensional electronic nature of Ta4SiTe4 by combining micro-spot angle-resolved photoemission spectroscopy and transport measurements on focused-ion-beam-processed samples. The angle-resolved photoemission spectroscopy measurements reveal anisotropic band dispersions along and perpendicular to the crystallographic c axis. Consistently, transport measurements demonstrate that the resistivity perpendicular to the c axis is approximately five times larger than that along the c axis at 200 K. These results provide direct experimental evidence for the quasi-one-dimensional electronic character of Ta4SiTe4, which underlies its giant thermoelectric response reported previously, and offer fundamental insights into the role of electronic dimensionality in enhancing thermoelectric performance.

cond-mat.mtrl-sci↗

arXiv2026

Molecular Orbital Degeneracy Lifting in a Tetrahedral Cluster System NbSeI

The lifting of degenerate electronic states, in which multiple electronic states share the same energy, is a fundamental issue in the physics of crystalline solids. In real materials, this problem has been extensively studied in transition metal compounds, where various quantum phenomena arise from the spin and orbital degeneracy of the d electrons on individual transition-metal atoms. In contrast, materials containing high-symmetry clusters composed of multiple transition-metal atoms are expected to exhibit more emergent phenomena due to the entanglement of the electronic degrees of freedom across multiple atoms. Here, we report the discovery of two distinct mechanisms of orbital-degeneracy lifting in NbSeI, which comprises Nb4 tetrahedral clusters with molecular orbital degrees of freedom and whose average crystal structure is predicted to host a flat-band metal. Below 106 K, NbSeI is found to be a nonmagnetic molecular orbital-ordered insulator. Above this temperature, the average structure becomes face-centered cubic without any superlattice, while the orbital degeneracy remains lifted by significant local distortions of Nb4 tetrahedra, which may be associated with a molecular orbital-liquid or orbital-frozen state. This noncooperative Jahn-Teller distortion stabilizes a nonmagnetic insulating state above 106 K, in stark contrast to the flat-band metal predicted from the average structure.

cond-mat.str-el↗

arXiv2025

Muon Knight shift as a precise probe of the superconducting symmetry of Sr$_2$RuO$_4$

Muon spin rotation ($\mu$SR) measurements of internal magnetic field shifts, known as the muon Knight shift, is used for determining pairing symmetries in superconductors. While this technique has been especially effective for $f$-electron-based heavy-fermion superconductors, it remains challenging in $d$-electron-based superconductors such as Sr$_2$RuO$_4$, where the Knight shift is intrinsically small. Here, we report high-precision muon Knight shift measurements of superconducting Sr$_2$RuO$_4$. We observe that using multiple pieces of crystals, a common practice in $\mu$SR measurements, induces a substantial paramagnetic shift below the superconducting transition temperature, $T_c$, when a weak magnetic field is applied. We attribute such an unresolved paramagnetic shift to stray fields generated by neighboring diamagnetic crystals. To avoid this, one piece of crystal was used in this study. We experimentally determine the muon Knight shift of Sr$_2$RuO$_4$ in the normal state to be -116$\pm$7 ppm. By combining the observed muon Knight shift with independently determined bulk magnetization data from the same crystal used in $\mu$SR and carefully separating various contributions to the shift, we confirm a significant reduction in the spin Knight shift below $T_c$, consistent with spin-singlet-like pairing. This result constitutes the precise muon Knight shift measurement in a $d$-electron-based superconductor. Our results highlight the potential of $\mu$SR as a powerful complementary technique to the established method of nuclear magnetic resonance for probing the spin susceptibility in superconductors.

cond-mat.supr-con↗

arXiv2025

From continuum excitations to sharp magnons via transverse magnetic field in the spin-1/2 Ising-like triangular lattice antiferromagnet Na2BaCo(PO4)2

We report high-resolution inelastic neutron scattering measurements of the excitation spectrum in large single crystals of the spin-1/2 triangular lattice Ising-like antiferromagnet Na2BaCo(PO4)2 in magnetic fields applied transverse to the Ising axis. In the high-field polarized phase above a critical field $B_{C}$ we observe sharp magnons, as expected in the case of no exchange disorder. Through simultaneous fits to the dispersions including data in polarizing field along the Ising axis, we obtain an excellent match to an Ising-like XXZ Hamiltonian and rule out previously proposed Kitaev exchanges. In the intermediate-field phase below $B_{C}$, we observe three dispersive modes, out of which only the lowest energy one is sharp and the others are broad and overlap with continuum scattering. We propose that the broadening effects are due to magnon decays into two-magnon excitations and confirm that such processes are kinematically allowed. The continuum scattering becomes progressively stronger upon lowering field and, at 0.25 T and zero field, it dominates the complete spectrum with no clear evidence for even broadened magnon modes. We discuss the relevance of the continuous manifold of mean-field degenerate ground states of the refined Hamiltonian for capturing the observed spectrum in zero field, and compare the data with the one- and two-magnon spectrum averaged over this manifold. We also propose a model of the interlayer couplings to explain the observed finite interlayer magnetic propagation vector of the zero-field magnetic order; this requires the breaking of the mirror symmetry in the nominal P-3m1 space group and through refinement of x-ray diffraction data on an untwinned single crystal, we indeed confirm a rotation of the CoO6 octahedra around the c-axis, which lowers the symmetry to P-3.

cond-mat.str-el↗

arXiv2025

Superconductivity in Ternary Zirconium Telluride Zr6RuTe2

Zr6CoAl2-type Zr6RuTe2 is found to show bulk superconductivity below the superconducting transition temperature Tc = 1.1 K, according to the electrical resistivity, magnetization, and heat capacity measurements using synthesized polycrystalline samples. This Tc exceeds that of Zr6MTe2 compounds in which M is other transition metals, indicating that M = Ru is favorable for superconductivity in Zr6CoAl2-type Zr6MX2.

cond-mat.supr-con↗

arXiv2025

Cubic ReSTe as a High-Performance Thermoelectric Material

We report thermoelectric properties of sintered samples of undoped, W-doped, and Sb-doped ReSTe crystallized in a cubic MoSBr-type structure. All samples exhibited p-type thermoelectric properties. ReSTe and Re0.993W0.007STe exhibited the largest dimensionless figure of merit ZT, reaching 0.4 at 660 K. This high performance is attributed to large power factor owing to the degenerate semiconducting state realized by the strong spin-orbit coupling and low lattice thermal conductivity of the sintered samples. Furthermore, electronic band dispersion of ReSTe is almost flat at the bottom of the conduction band, suggesting that n-type ReSTe is expected to exhibit much higher performance than p-type ReSTe.

cond-mat.mtrl-sci↗

arXiv2024

Topological Semimetal KAlGe with Novel Electronic Instability

Compounds with the anti-PbFCl structure exhibit a variety of electronic instabilities and intriguing physical properties. NaAlSi and NaAlGe are similar topological nodal-line semimetals, but they have distinct properties. NaAlSi is a superconductor at 6.8 K, whereas NaAlGe is an insulator with a pseudogap of approximately 100 K. Using the potassium-indium flux method, we succeeded in synthesizing a single crystal of KAlGe, a new anti-PbFCl compound. First principles electronic structure calculations reveal that KAlGe is isoelectronic with NaAlSi and NaAlGe. KAlGe undergoes a metal-to-metal transition at 89 K and exhibits no superconductivity above 1.8 K. The low temperature phase has significantly lower carrier density and extremely high mobility, similar to Dirac electron systems. Furthermore, X-ray diffraction experiments show a structural change that breaks the fourfold symmetry during the phase transition. Electron-phonon interactions may be responsible for superconductivity in NaAlSi, whereas excitonic electron-hole interactions are thought to play an important role in KAlGe and possibly NaAlGe. Our findings demonstrate that fascinating physics lies within the compound family.

cond-mat.str-el↗

arXiv2024

Superconductivity in Hexagonal Zr6CoAl2-Type Zr6RuBi2 and Zr6FeBi2

We report the synthesis and electronic properties of polycrystalline samples of Zr6MBi2 (M = Ru and Fe) crystallizing in the hexagonal Zr6CoAl2-type structure. Based on their electrical resistivity, magnetization, and heat capacity data, Zr6RuBi2 and Zr6FeBi2 are found to exhibit bulk superconductivity below Tc = 4.9 and 1.4 K, respectively. Although Zr6RuBi2 is most likely a conventional superconductor, the considerably higher Tc for M = Ru than that for M = Fe differs from the trend in Tc for Zr6CoAl2-type superconductors reported thus far. The superconductivity of an amorphous solid-solution phase, which may hinder elucidation of the superconducting properties of Zr6MBi2, is also discussed.

cond-mat.supr-con↗

arXiv2024

Compass-model physics on the hyperhoneycomb lattice in the extreme spin-orbit regime

The physics of spin-orbit entangled magnetic moments of $4d$ and $5d$ transition metal ions on a honeycomb lattice has been much explored in search for unconventional magnetic orders or quantum spin liquids expected for compass spin models, where different bonds in the lattice favour different orientations for the magnetic moments. Realizing such physics with rare-earth ions is a promising route to achieve exotic ground states in the extreme spin orbit limit, however this regime has remained experimentally largely unexplored due to major challenges in materials synthesis. Here we report successful synthesis of powders and single crystals of $β$-Na$_2$PrO$_3$, with $4f^{1}$ Pr$^{4+}$ $j_\mathrm{eff}\!=\!1/2$ magnetic moments arranged on a hyperhoneycomb lattice with the same threefold coordination as the planar honeycomb. We find a strongly noncollinear magnetic order with highly dispersive gapped excitations that we argue arise from frustration between bond-dependent, anisotropic off-diagonal exchanges, a compass quantum spin model not explored experimentally so far. Our results show that rare-earth ions on threefold coordinated lattices offer a platform for the exploration of quantum compass spin models in the extreme spin orbit regime, with qualitatively distinct physics from that of $4d$ and $5d$ Kitaev materials.

cond-mat.str-el↗

arXiv2024

Selective synthesis and crystal chemistry of candidate rare earth Kitaev materials: honeycomb and hyperhoneycomb Na$_2$PrO$_3$

Rare earth oxides have attracted interest as a platform for studying frustrated magnetism arising from bond dependent anisotropic interactions. Ordered rock salt compounds Na$_2$PrO$_3$ crystallize in two polymorphs ($α$ and $β$) comprising honeycomb and hyperhoneycomb lattices of octahedrally coordinated Pr$^{4+}$ (4$f^1$). Although possible realization of antiferromagnetic Kitaev interactions is anticipated for these phases on the basis of ab initio models, the air-sensitivity of the two polymorphs has hampered reliable crystal growth and physical property measurements. Here, we have succeeded in preparing powder and single crystals of both $α$- and $β$-Na$_2$PrO$_3$ using modified synthetic procedures. Revised crystal structures for both polymorphs are obtained from refinement of untwinned single-crystal X-ray diffraction data.

cond-mat.str-el↗

arXiv2024

Superconductivity in Ternary Zirconium Telluride Zr6MTe2 with 3d Transition Metals

We report the synthesis, electronic properties, and electronic states of Zr6MTe2 (M = Cr, Mn, Fe, and Co), which is isostructural to a recently discovered superconductor family Sc6MTe2. Based on the electrical resistivity and heat capacity data measured at low temperatures, Zr6FeTe2 is found to show bulk superconductivity below Tc = 0.76 K. Zr6CoTe2 also exhibited zero resistivity due to superconductivity below 0.13 K. In contrast, Zr6+dMn1-dTe2 does not show superconductivity but instead exhibits strong magnetism, which most likely prevents the formation of superconductivity in this material. The electronic properties and electronic states of Zr6MTe2 are discussed in comparison with those of Sc6MTe2.

cond-mat.supr-con↗

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

Magnetic frustration in a van der Waals metal CeSiI

The realization of magnetic frustration in a metallic van der Waals (vdW) coupled material has been sought as a promising platform to explore novel phenomena both in bulk matter and in exfoliated devices. However, a suitable material platform has been lacking so far. Here, we demonstrate that CeSiI hosts itinerant electrons coexisting with exotic magnetism. In CeSiI, the magnetic cerium atoms form a triangular bilayer structure sandwiched by van der Waals stacked iodine layers. From resistivity and magnetometry measurements, we confirm the coexistence of itinerant electrons with magnetism with dominant antiferromagnetic exchange between the strongly Ising-like Ce moments below 7 K. Neutron diffraction directly confirms magnetic order with an incommensurate propagation vector k ~ (0.28, 0, 0.19) at 1.6 K, which points to the importance of further neighbor magnetic interactions in this system. The presence of a two-step magnetic-field-induced phase transition along c axis further suggests magnetic frustration in the ground state. Our findings provide a novel material platform hosting a coexistence of itinerant electron and frustrated magnetism in a vdW system, where exotic phenomena arising from rich interplay between spin, charge and lattice in low dimension can be explored.

cond-mat.str-el↗

arXiv2021

Dimensional reduction by geometrical frustration in a cubic antiferromagnet composed of tetrahedral clusters

Dimensionality is a critical factor in determining the properties of solids and is an apparent built-in character of the crystal structure. However, it can be an emergent and tunable property in geometrically frustrated spin systems. Here, we study the spin dynamics of the tetrahedral cluster antiferromagnet, pharmacosiderite, via muon spin resonance and neutron scattering. We find that the spin correlation exhibits a two-dimensional characteristic despite the isotropic connectivity of tetrahedral clusters made of spin 5/2 Fe3+ ions in the three-dimensional cubic crystal, which we ascribe to two-dimensionalisation by geometrical frustration based on spin wave calculations. Moreover, we suggest that even one-dimensionalisation occurs in the decoupled layers, generating low-energy and one-dimensional excitation modes, causing large spin fluctuation in the classical spin system. Pharmacosiderite facilitates studying the emergence of low-dimensionality and manipulating anisotropic responses arising from the dimensionality using an external magnetic field.

cond-mat.str-el↗

arXiv2020

Magnetization Plateau Observed by Ultra-High Field Faraday Rotation in a Kagomé Antiferromagnet Herbertsmithite

To capture the high-field magnetization process of herbertsmithite (ZnCu3(OH)6Cl2), Faraday rotation (FR) measurements were carried out on a single crystal in magnetic fields of up to 190 T. The magnetization data evaluated from the FR angle exhibited a saturation behavior above 150 T at low temperatures, which was attributed to the 1/3 magnetization plateau. The overall behavior of the magnetization process was reproduced by theoretical models based on the nearest-neighbor Heisenberg model. This suggests that herbertsmithite is a proximate kagome antiferromagnet hosting an ideal quantum spin liquid in the ground state. A distinguishing feature is the superlinear magnetization increase, which is in contrast to the Brillouin function-type increase observed by conventional magnetization measurements and indicates a reduced contribution from free spins located at the Zn sites to the FR signal.

cond-mat.str-el↗