arXiv subjects

Tsuyoshi Kimura

Publications and source records attributed to Tsuyoshi Kimura.

At least 19 recordsLinked to original sources

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

Raman Optical Activity Induced by Ferroaxial Order in NiTiO$_3$

Raman optical activity (ROA), the dependence of Raman intensity on the circular polarization of incident and scattered light, has traditionally been observed in chiral molecules and magnetic materials, where inversion or time-reversal symmetry is broken. Here we demonstrate that ROA can also arise in a centrosymmetric and non-magnetic ferroaxial crystal. Using circularly polarized Raman spectroscopy on single-crystalline NiTiO$_3$, we observed a pronounced ROA signal in the cross-circular polarization configurations, which correlates with the ferroaxial domain structure. Our symmetry analysis, first-principles calculations of phonons, and tight-binding model calculations reveal that the natural ROA originates from the ferroaxial order and persists even within the electric dipole approximation. These results establish ROA as a powerful probe of ferroaxial order in centrosymmetric systems.

cond-mat.mtrl-sci↗

arXiv2026

Electric-field-induced X-ray Nonreciprocal Dichroism in Hematite

Hematite (alpha-Fe2O3) is a prototypical room temperature antiferromagnet whose time-reversal-odd magnetic structure has recently attracted renewed attention. While such magnetic symmetry can be characterized in terms of higher-order multipoles beyond the magnetic dipole, their manifestation in measurable physical phenomena has remained largely elusive. In this work, we investigate x-ray absorption near the Fe K-edge of hematite under an applied electric field, which explicitly breaks space-inversion symmetry. We observe an electric-field-induced x-ray nonreciprocal linear dichroism (E-induced XNLD) that reflects the time-reversal-odd nature of the magnetic order. Numerical simulations based on ab-initio density functional theory reproduce the observed spectra, including their dependence on the antiferromagnetic domain and x-ray polarization. Furthermore, a symmetry-resolved multipole analysis reveals that this response originates from the magnetic quadrupole and the magnetic toroidal octupole induced by the applied electric field. These results demonstrate that electric-field-modulated x-ray absorption provides direct access to the antiferroic order of higher-order multipoles in time-reversal-odd antiferromagnets, thereby establishing a general framework to uncover hidden symmetry properties in magnetic materials.

cond-mat.mtrl-sci↗

arXiv2026

Magnetoelectric training of multiferroic domains in Mn$_2$GeO$_4$

Magnetoelectric multiferroics promise direct cross-control between coexisting ferroelectric and ferromagnetic orders, which is of interest for applications in magnetism and spintronics. A particularly interesting type of cross-control is found in spin-spiral multiferroic Mn$_2$GeO$_4$, where a ferroelectric multi-domain distribution can be globally inverted by a single magnetic field sweep. In this work we consider the initial domain evolution from zero-field cooling, imaging the evolution of domains under both magnetic and electric fields via optical second harmonic generation. We find that polarization and magnetization domains form independently when entering the multiferroic phase, and a single deterministic initialisation procedure, spanning three quarters of a field cycle, is required to achieve reliable magnetoelectric cross-coupling. This initialisation behaviour originates from a deterministic pathway from metastable to equilibrium domain patterns, in contrast to more common and less reliable domain "training" procedures that require repeated field cycles. Understanding the initial domain evolution thus enables reliable cross-control in magnetoelectric devices with highly interlinked order parameters.

cond-mat.mtrl-sci↗

arXiv2026

Coupled sawtooth chain exchange network in olivine Mn$_2$GeO$_4$

Sawtooth chain magnets have been a subject of historical interest in the field of frustrated magnetism, with classical olivine family $M_2TX_4$, ($M$ - 3d, $T$ - 4p, $X$ - chalcogen elements) typically realizing simple $\mathbf{k} = (000)$ states. The magnetism of the Mn$_2$GeO$_4$ olivine is surprisingly complex, proceeding from commensurate states to a multiferroic commensurate + incommensurate phase. Here we report inelastic neutron scattering results from a Mn$_2$GeO$_4$ single crystal and develop an effective Hamiltonian including long-distance bilinear and dipolar interactions. The magnetic interactions are predominantly antiferromagnetic and span a three-dimensional exchange network consisting of coupled sawtooth chains. Based on the determined strength of the couplings, the dominant sawtooth chains appear at third- and fourth- rather than next-nearest-neighbor. However the next-nearest-neighbor interaction is, along with a modest Dzyaloshinskii-Moriya interaction, important for modeling the observed incommensurability. We use the best-fit Hamiltonian as the basis for Langevin dynamics simulations and Luttinger-Tisza calculations of the high-temperature commensurate transition.

cond-mat.str-el↗

arXiv2025

Raman Spectroscopic Investigation of Ferroaxial Order in Na2BaNi(PO4)2 Single Crystals

Ferroaxial order is characterized by the breaking of mirror symmetry parallel to the crystallographic principal axis, which often originates from spontaneous rotational distortions of the crystal lattice. Such rotational distortions are, by symmetry, allowed to couple to specific phonon modes. However, Raman-active phonons associated with these rotational distortions have not yet been clearly identified on a symmetry-consistent basis. Here, we perform polarization-resolved Raman spectroscopy on the ferroaxial phase of Na2BaNi(PO4)2 single crystals and combine the measurements with first-principles lattice-dynamics calculations. This symmetry-guided analysis enables a comprehensive assignment of Raman-active modes in the ferroaxial phase. Several low-frequency Ag modes exhibit finite linewidth broadening, suggesting that these phonons may be weakly affected by the underlying rotational distortion. These results establish a symmetry-based spectroscopic framework for analyzing phonons associated with rotational distortions in ferroaxial materials and provide a basis for future studies of ferroaxial order in complex oxides.

cond-mat.mtrl-sci↗

arXiv2025

Nonreciprocal charge transport in an iron-based superconductor with broken inversion symmetry engineered by a hydrogen-concentration gradient

The breaking of spatial inversion symmetry in condensed matter gives rise to intriguing physical properties, such as ferroelectricity, piezoelectricity, spin-momentum locking, and nonreciprocal responses. Here we propose that a concentration gradient, which often persists as a quasi-stable nonequilibrium state with long relaxation times in solids, can serve as a general platform for inversion symmetry breaking. We demonstrate this concept in an epitaxial thin film of the hydrogen-doped SmFeAsO (Sm1111:H) superconductor with a depthwise hydrogen-concentration gradient introduced via an optimized topotactic reaction. This film exhibits nonreciprocal charge transport, meaning that the electrical resistance depends on the direction of the applied current, which serves as a key signature of broken inversion symmetry. A pronounced nonreciprocal signal emerges in the vicinity of the superconducting transition, which we attribute to vortex-motion nonreciprocity arising from an asymmetric pinning landscape created by the hydrogen-concentration gradient. Owing to the high critical temperature of Sm1111:H, vortex-origin nonreciprocity is observed above 40 K, representing the highest temperature reported to date among single bulk materials without an artificially hetero-layered structure. Our findings establish concentration-gradient engineering as a versatile and broadly applicable route for realizing inversion-broken states in otherwise centrosymmetric hosts, opening pathways toward a broader landscape of odd-parity-driven functionalities.

cond-mat.mtrl-sci↗

arXiv2025

Electric-field-induced magnetic toroidal moment and nonlinear magnetoelectric effect in antiferromagnetic olivines

Beyond conventional electric and magnetic monopoles, electric and magnetic toroidal monopoles, which are rank-0 multipoles distinguished by opposite parities under spatial inversion and time reversal, can exist in nature. The recent observation of electric-field-induced directional dichroism in antiferromagnetic olivine Co$_2$SiO$_4$ has provided the first concrete example of a magnetic toroidal monopole; however, its microscopic origin remains elusive. Here, we propose a minimal spin model that incorporates magnetoelectric coupling via the $d$-$p$ hybridization mechanism and analyze it within the mean-field approximation. The model qualitatively reproduces the experimentally observed temperature dependence of the dielectric constant and its pronounced sensitivity to the direction of the applied electric field. Furthermore, it elucidates the temperature evolution of the magnetic toroidal monopole and the strong electric-field-direction dependence of the magnetic toroidal moment. Our calculations also predict a second-order nonlinear magnetoelectric response, consistent with the symmetry classification of Co$_2$SiO$_4$ as an altermagnet. Additionally, we demonstrate that the same framework is applicable to other antiferromagnetic olivines with analogous magnetic order, indicating the robustness and generality of the toroidal-type magnetoelectric response in this material family.

cond-mat.str-el↗

arXiv2025

Broad Spectral Tuning of Ultra-Low Loss Polaritons in a van der Waals Crystal by Intercalation

Phonon polaritons (PhPs) -- light coupled to lattice vibrations -- in polar van der Waals (vdW) crystals are promising candidates for controlling the flow of energy at the nanoscale due to their strong field confinement, anisotropic propagation, and ultra-long lifetime in the picosecond range \cite{ref1,ref2,ref3,ref4,ref5}. However, the lack of tunability in their narrow and material-specific spectral range -- the Reststrahlen Band (RB) -- severely limits their technological implementation. Here, we demonstrate that the intercalation of Na atoms in the vdW semiconductor $α$-V$_2$O$_5$ enables a broad spectral shift of RBs, and that the PhPs excited exhibit ultra-low losses (lifetime of $4 \pm 1$~ps), similar to PhPs in the non-intercalated crystal (lifetime of $6 \pm 1$ ps). We expect our intercalation method to be applicable to other vdW crystals, opening the door for the use of PhPs in broad spectral bands in the mid-infrared domain.

physics.optics↗

arXiv2024

Electric field-induced nonreciprocal directional dichroism in a time-reversal-odd antiferromagnet

Antiferromagnets with broken time-reversal (T) symmetry (T-odd antiferromagnets) have gained extensive attention, mainly due to their ferromagnet-like behavior despite the absence of net magnetization. However, certain types of T-odd antiferromagnets remain inaccessible by the typical ferromagnet-like phenomena (e.g., anomalous Hall effect). One such system is characterized by a T-odd scalar quantity, the magnetic toroidal monopole. To access the broken T symmetry in such a system, we employ a unique nonreciprocal optical phenomenon, electric field-induced nonreciprocal directional dichroism (E-induced NDD). We successfully detected signals of E-induced NDD in a T-odd antiferromagnet, Co2SiO4, whose magnetic structure is characterized by the magnetic toroidal monopole. Furthermore, by spatially resolving the E-induced NDD, we visualized spatial distributions of a pair of domain states related to one another by the T operation. The domain imaging revealed the inversion of the domain pattern by applying a magnetic field, which is explained by trilinear coupling attributed to the piezomagnetic effect. Our observation of E-induced NDD provides a unique approach to accessing the order parameter in T-odd antiferromagnets.

cond-mat.mtrl-sci↗

arXiv2024

Spin dynamics in linear magnetoelectric material Mn$_{3}$Ta$_{2}$O$_{8}$

We performed inelastic neutron scattering experiments on single crystal samples of a linear magnetoelectric material Mn$_{3}$Ta$_{2}$O$_{8}$, which exhibits a collinear antiferromagnetic order, to reveal the spin dynamics. Numerous modes observed in the neutron spectra were reasonably reproduced by linear spin-wave theory on the basis of the spin Hamiltonian including eight Heisenberg interactions and an easy-plane type single-ion anisotropy. The presence of strong frustration was found in the identified spin Hamiltonian.

cond-mat.str-el↗

arXiv2023

High-field phase diagram of the chiral-lattice antiferromagnet Sr(TiO)Cu4(PO4)4

High-field phase diagram of a chiral-lattice antiferromagnet Sr(TiO)Cu4(PO4)4 is studied by means of the ultrasound, dielectric, and magnetocaloric-effect measurements. These experimental techniques reveal two new phase transitions at high fields, which have not been resolved by the previous magnetization experiments. Specifically, the c66 acoustic mode shows drastic changes with hysteresis with applied fields along the c axis, indicating a strong magneto-elastic coupling. Combined with the cluster mean-field theory, we discuss the origins of these phase transitions. By considering the chiral-twist effect of Cu4O12 cupola units, which is inherent to the chiral crystal structure, the phase diagram is reasonably reproduced. The agreement between the experiment and theory suggests that this material is a unique quasi two-dimensional spin system with competing exchange interactions and chirality, leading to the rich phase diagram.

cond-mat.str-el↗

arXiv2023

Non-equilibrium dynamics of spin-lattice coupling

Interactions between the different degrees of freedom form the basis of many manifestations of intriguing physics in condensed matter. In this respect, quantifying the dynamics of normal modes that themselves arise from these interactions and how they interact with other excitations is of central importance. Of the different types of coupling that are often important, spin-lattice coupling is relevant to several sub-fields of condensed matter physics; examples include spintronics, high-TC superconductivity, and topological materials. While theories of materials where spin-lattice coupling is relevant can sometimes be used to infer the magnitude and character of this interaction, experimental approaches that can directly measure it are rare and incomplete. Here we use time-resolved X-ray diffraction to directly access the spin-lattice coupling by measuring both ultrafast atomic motion and the associated spin dynamics following the excitation of a coherent electromagnon by an intense THz pulse in a multiferroic hexaferrite. Comparing the dynamics of the two different components, one striking outcome is the different phase shifts relative to the driving field. This phase shift provides insight into the excitation process of such a coupled mode. This direct observation of combined lattice and magnetization dynamics paves the way to access the mode-selective spin-lattice coupling strength, which remains a missing fundamental parameter for ultrafast control of magnetism and is relevant to a wide variety of correlated electron physics.

cond-mat.str-el↗

arXiv2022

Ferroelectric transition of a chiral molecular crystal BINOL2DMSO

We report dielectric, thermodynamical, acoustic, and optical properties of a chiral molecular crystal, 1,1'-bi-2-naphthol 2-dimethylsulfoxide (BINOL2DMSO). We find two successive phase transitions at Tc1=190 K and Tc2=125 K. The first transition at Tc1 is characterized by an order-disorder transition of the guest molecules DMSO along with ferroelectricity. At the second transition of Tc2, the crystal structure deforms from tetragonal to monoclinic, leading to domain formation. Low-temperature x-ray diffraction suggests that the space group changes from P4_12_12 (P4_32_12) to P4_1 (P4_3) at Tc1, and down to P112_1 at Tc2.

cond-mat.mtrl-sci↗

arXiv2022

Spin dynamics in the square-lattice cupola system Ba(TiO)Cu$_4$(PO$_4$)$_4$

We report high-resolution single-crystal inelastic neutron scattering measurements on the spin-1/2 antiferromagnet Ba(TiO)Cu$_4$(PO$_4$)$_4$. This material is formed from layers of four-site \cupola" structures, oriented alternately upwards and downwards, which constitute a rather special realization of two-dimensional (2D) square-lattice magnetism. The strong Dzyaloshinskii-Moriya (DM) interaction within each cupola, or plaquette, unit has a geometry largely unexplored among the numerous studies of magnetic properties in 2D Heisenberg models with spin and spatial anisotropies. We have measured the magnetic excitations at zero field and in fields up to 5 T, finding a complex mode structure with multiple characteristic features that allow us to extract all the relevant magnetic interactions by modelling within the linear spin-wave approximation. We demonstrate that Ba(TiO)Cu$_4$(PO$_4$)$_4$ is a checkerboard system with almost equal intra- and inter-plaquette couplings, in which the intra-plaquette DM interaction is instrumental both in enforcing robust magnetic order and in opening a large gap at the Brillouin-zone center. We place our observations in the perspective of generalized phase diagrams for spin-1/2 square-lattice models and materials, where exploring anisotropies and frustration as routes to quantum disorder remains a frontier research problem.

cond-mat.str-el↗

arXiv2021

Optical excitation of electromagnons in hexaferrite

Understanding ultrafast magnetization dynamics on the microscopic level is of strong current interest due to the potential for applications in information storage. In recent years, the spin-lattice coupling has been recognized to be essential for ultrafast magnetization dynamics. Magnetoelectric multiferroics of type II possess intrinsic correlations among magnetic sublattices and electric polarization (P) through spin-lattice coupling, enabling fundamentally coupled dynamics between spins and lattice. Here we report on ultrafast magnetization dynamics in a room-temperature multiferroic hexaferrite possessing ferrimagnetic and antiferromagnetic sublattices, revealed by time-resolved resonant x-ray diffraction. A femtosecond above-bandgap excitation triggers a coherent magnon in which the two magnetic sublattices entangle and give rise to a transient modulation of P. A novel microscopic mechanism for triggering the coherent magnon in this ferrimagnetic insulator based on the spin-lattice coupling is proposed. Our finding opens up a novel but general pathway for ultrafast control of magnetism.

cond-mat.str-el↗

arXiv2020

Capacitive detection of magnetostriction, dielectric constant, and magneto-caloric effects in pulsed magnetic fields

We report on the development of a capacitance measuring system which allows measurements of capacitance in pulsed magnetic fields up to 61~T. By using this system, magnetic-field responses of various physical quantities such magnetostriction, magnetic-field-induced change in complex dielectric constant, and magneto-caloric effect can be investigated in pulsed-magnetic-field conditions. Here, we examine the validity of our system for investigations of these magnetic-field-induced phenomena in pulse magnets. For the magnetostriction measurement, magnetostriction of a specimen can be measured through a change in the capacitance between two aligned electrodes glued on the specimen and a dilatometer. We demonstrate a precise detection of valley polarization in semimetallic bismuth through a magnetostriction signal with a resolution better than 10$^{-6}$ of the relative length change. For the magnetic-field-induced change in complex dielectric constant, we successfully observed clear dielectric anomalies accompanied by magnetic/magnetoelectric phase transitions in multiferroic Pb(TiO)Cu$_4$(PO$_4$)$_4$. For the measurement of magneto-caloric effect, a magnetic-field-induced change in sample temperature was verified for Gd$_3$Ga$_5$O$_{12}$ with a capacitance thermometer made of a non-magnetic ferroelectric compound KTa$_{1-x}$Nb$_x$O$_3$ ($x$ = 0.02) whose capacitance is nearly field-independent. These results show that our capacitance measuring system is a promising tool to study various magnetic-field-induced phenomena which have been difficult to detect in pulsed magnetic fields.

cond-mat.str-el↗

arXiv2020

Domain switching and exchange bias control by electric field in multiferroic conical magnet Mn$_2$GeO$_4$

The electric field effect on magnetism was examined in the multiferroic conical magnet Mn$_2$GeO$_4$, which shows a strong coupling between ferromagnetic and ferroelectric order parameters. The systematic evaluation of the electric polarization in the multiferroic phase below 5.5 K under various field cooling conditions reveals that small magnetic fields of 0.1 T significantly reduce the required electric fields needed to reach saturation. By applying electric fields during magnetic field dependent hysteresis measurements of magnetization M and polarization P an electrically controllable exchange bias was observed, a phenomenon exceedingly rare in single phase multiferroics. Furthermore, non-reversible electric switching of P and M domains was achieved under specific magnetic field conditions.

cond-mat.str-el↗