arXiv subjects

Kenta Kimura

Publications and source records attributed to Kenta Kimura.

At least 19 recordsLinked to original sources

arXiv2026

Optical switching of antiferromagnetic domains by nonreciprocal heat current

What distinguishes front from back? In physics, such directionality emerges only when an underlying symmetry is broken. Antiferromagnets that inherently break both space-inversion and time-reversal symmetries provide a striking example, exhibiting nonreciprocal optical responses that depend on the direction of light propagation. Beyond distinguishing antiferromagnetic domains, we show that this nonreciprocity can deterministically create them. Using mid-infrared light, we demonstrate deterministic switching of antiferromagnetic domains in the magnetoelectric antiferromagnet LiFePO4, where illumination from opposite sides selectively stabilizes opposite domain states. Remarkably, the switching persists over a broad wavelength range rather than being confined to a narrow transition-specific spectral region, overcoming the spectral and material constraints of resonance-based optical switching schemes. The broadband switching originates from the material's intrinsic nonreciprocity through optically generated heat currents. Our results establish nonreciprocity as a general principle for deterministically controlling symmetry-broken phases with light.

cond-mat.str-el↗

arXiv2026

Single-crystal growth and magnetic, magnetoelectric, and optical properties of ferroaxial-type SrMn$_2$Ni$_6$Te$_3$O$_{18}$

Single crystals of SrMn$_2$Ni$_6$Te$_3$O$_{18}$, a member of the ferroaxial-type magnetic oxide family $AB_{2}C_{6}$Te$_3$O$_{18}$ ($A$ = Pb, Sr; $B$ = Mn, Cd; $C$ = Ni, Co), have been successfully grown, and their structural, magnetic, magnetoelectric, and optical properties have been systematically studied. Imaging of the spatial distribution of electric-field-induced optical rotation reveals that the single crystals preferentially form single ferroaxial (FA) domains. Magnetization and neutron diffraction measurements show that Mn$^{2+}$ and Ni$^{2+}$ magnetic moments order antiferromagnetically at $T_{\rm N}$ = 83 K, forming a $c$-axis collinear bidirector-type antiferromagnetic structure. All independent magnetoelectric tensor components allowed by the magnetic point group 6/$m^{\prime}$ have been detected, and the $χ_{33}$ component exhibits a pronounced temperature-dependent anomaly, including a peak and a sign reversal. Preferential formation of single FA domains and a similar $χ_{33}$ anomaly are also observed in the isostructural compound PbMn$_2$Ni$_6$Te$_3$O$_{18}$. These findings suggest that the ferroaxial and magnetic characteristics within this structural framework are robust against Sr-Pb replacement.

cond-mat.mtrl-sci↗

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

Magnetic-field switching of exciton-magnon coupling in LiNiPO$_4$

Exciton-magnon transitions provide a fundamental optical fingerprint of coupled excitonic and magnetic excitations in antiferromagnets. However, controlling such coupled excitations by external fields remains a key challenge. Here we report the temperature and magnetic-field evolution of exciton-magnon coupling in the magnetoelectric antiferromagnet LiNiPO$_4$ using pulsed magnetic fields up to 50 T. The magnon sideband intensity exhibits sharp switching across field-induced magnetic phases, with strong suppression in plateau phases and enhancement in canted spin states. This behavior is attributed to the interplay between the thermal magnon population and the spin-dependent optical transition matrix element. These results demonstrate that magnetic-field control of spin degrees of freedom enables selective switching of exciton-magnon coupling in antiferromagnets.

cond-mat.str-el↗

arXiv2026

Realization of a triangular spin necklace in a verdazyl-based Ni complex

We successfully synthesized a verdazyl-based complex, ($m$-Py-V)$_3$[Ni(NO$_3$)$_2$], in which Ni$^{2+}$ ions and verdazyl radicals form a one-dimensional, triangular spin necklace consisting of spin-1/2 and spin-1 units. Molecular orbital calculations reveal strong antiferromagnetic (AF) interactions between inversion-related radical pairs that form spin-1/2 singlet dimers. The remaining verdazyl and Ni$^{2+}$ spins form frustrated triangular units, creating a distinctive spin network. Magnetic susceptibility and specific heat measurements identify a phase transition to an AF order. The application of magnetic fields suppresses the phase transition signal, suggesting field-induced decoupling of the spin-1 moments. Electron spin resonance measurements are used to evaluate the easy-axis anisotropy of spin-1, which may promote the AF order. This work provides a rare example of a geometrically frustrated quantum spin chain realized via molecular design, thereby offering a platform for exploring frustration-driven quantum phases in low-dimensional materials.

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

Spin polarization driven by molecular vibrations leads to enantioselectivity in chiral molecules

Chirality pervades multiple scientific domains-physics, chemistry, biology, and astronomy-and profoundly influences their foundational principles. Recently, the chirality-induced spin selectivity (CISS) phenomenon has captured significant attention in physical chemistry due to its potential applications and intriguing underlying physics. Despite its prominence, the microscopic mechanisms of CISS remain hotly debated, hindering practical applications and further theoretical advancements. Here we challenge the established view that attributes CISS-related phenomena to current-induced spin polarization and electron transport across interfaces. We propose that molecular vibrations in chiral molecules primarily drive spin polarization, thereby governing CISS. Employing an electrochemical cell paired with a precisely engineered magnetic multilayer, we demonstrate that the magnetic interactions akin to interlayer exchange coupling are crucial for CISS. Our theoretical study suggests that molecular vibrations facilitate chirality-dependent spin polarization, which plays a pivotal role in CISS-related phenomena such as magnetoresistance and enantiomer separation using ferromagnets. These findings necessitate a paradigm shift in the design and analysis of systems in various scientific fields, extending the role of spin dynamics from traditional areas such as solid-state physics to chemical reactions, molecular biology, and even drug discovery.

cond-mat.mtrl-sci↗

arXiv2024

Observation of converse flexoelectric effect in topological semimetals

A strong coupling between electric polarization and elastic deformation in solids is an important factor in creating useful electromechanical nanodevices. Such coupling is typically allowed in insulating materials with inversion symmetry breaking as exemplified by the piezoelectric effect in ferroelectric materials. Therefore, materials with metallicity and centrosymmetry have tended to be out of scope in this perspective. Here, we report the observation of giant elastic deformation by the application of an alternating electric current in topological semimetals (V,Mo)Te2, regardless of the centrosymmetry. Considering the crystal and band structures and the asymmetric measurement configurations in addition to the absence of the electromechanical effect in a trivial semimetal TiTe2, the observed effect is discussed in terms of a Berry-phase-derived converse flexoelectric effect in metals. The observation of the flexoelectric effect in topological semimetals paves a way for a new type of nanoscale electromechanical sensors and energy harvesting.

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↗

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↗

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↗

arXiv2019

Magnetic structure in square cupola compound Ba(TiO)Cu$_4$(PO$_4$)$_4$: a $^{31}$P NMR Study

The magnetic structure of the antiferromagnetic square cupola compound Ba(TiO)Cu$_4$(PO$_4$)$_4$ with the tetragonal structure is studied with 31P nuclear magnetic resonance techniques. The magnetic hyperfine shift K shows a clear splitting at the Néel temperature T$_N$ = 9.5 K, where the resonance splits into two lines when an external magnetic field is oriented along the c axis and into four lines when the field is along the a axis. In the paramagnetic region K(T) follows temperature dependence of the magnetic susceptibility $χ(T)$. From K vs $χ$ plot we determined nearly isotropic hyperfine field values Ha_hf = 765 mT/$μ_B$ and Hc_hf = 740 mT/$μ_B$ for the magnetic field oriented along a and c, respectively. From the rotation of the single crystal in the external magnetic field we determined eight different orientations of K-tensor in the paramagnetic region. In the antiferromagnetic state at T = 6 K we found that the local field at phosphorus is mainly due to dipolar field of coppers. Here the rotation of the single crystal shows eight different orientations of the local field Bint = 35.6 mT. The orientations correspond to the calculation of dipolar fields at phosphorus assuming magnetic quadrupolar configuration of magnetic moments $\varGamma_3(1)$ described previously [Nat. Commun. 7, 13039 (2016); Phys. Rev. B 96, 214436 (2017)].

cond-mat.str-el↗

arXiv2018

Magnetoelectric behavior from cluster multipoles in square cupolas: Study of Sr(TiO)Cu$_4$(PO$_4$)$_4$ in comparison with Ba and Pb isostructurals

We report our combined experimental and theoretical study of magnetoelectric properties of an antiferromagnet Sr(TiO)Cu$_4$(PO$_4$)$_4$, in comparison with the isostructurals Ba(TiO)Cu$_4$(PO$_4$)$_4$ and Pb(TiO)Cu$_4$(PO$_4$)$_4$. The family of compounds commonly possesses a low-symmetric magnetic unit called the square cupola, which is a source of magnetoelectric responses associated with the magnetic multipoles activated under simultaneous breaking of spatial inversion and time reversal symmetries. Measuring the full magnetization curves and the magnetic-field profiles of dielectric constant for Sr(TiO)Cu$_4$(PO$_4$)$_4$ and comparing them with the theoretical analyses by the cluster mean-field theory, we find that the effective $S=1/2$ spin model, which was used for the previous studies for Ba(TiO)Cu$_4$(PO$_4$)$_4$ and Pb(TiO)Cu$_4$(PO$_4$)$_4$, well explains the experimental results by tuning the model parameters. Furthermore, elaborating the phase diagram of the model, we find that the square cupolas could host a variety of magnetic multipoles, i.e., monopole, toroidal moment, and quadrupole tensor, depending on the parameters that could be modulated by deformations of the magnetic square cupolas. Our results not only provide a microscopic understanding of the series of the square cupola compounds, but also stimulate further exploration of the magnetoelectric behavior arising from cluster multipoles harboring in low-symmetric magnetic units.

cond-mat.str-el↗

arXiv2018

Magnetic Structural Unit with Convex Geometry: a Building Block Hosting an Exchange-striction-driven Magnetoelectric Coupling

We perform a combined experimental and theoretical study of a magnetic-field ($B$) induced evolution of magnetic and ferroelectric properties in an antiferromagnetic material Pb(TiO)Cu$_4$(PO$_4$)$_4$, whose structure is characterized by a staggered array of Cu$_4$O$_{12}$ magnetic units with convex geometry known as square cupola. Our experiments show a $B$-induced phase transition from a previously reported low-$B$ linear magnetoelectric phase to a new high-$B$ magnetoelectric phase, which accompanies a 90$^\circ$ flop of electric polarization and gigantic magnetodielectric effect. Moreover, we observe a $B$-induced sign reversal of ferroelectric polarization in the high-$B$ phase. Our model and first-principles calculations reveal that the observed complex magnetoelectric behavior is well explained in terms of a $B$-dependent electric polarization generated in each Cu$_4$O$_{12}$ unit by the so-called exchange striction mechanism. The present study demonstrates that the materials design based on the magnetic structural unit with convex geometry deserves to be explored for developing strong magnetoelectric couplings.

cond-mat.mtrl-sci↗

arXiv2017

Frustrated magnetism in the Heisenberg pyrochlore antiferromagnets $A$Yb$_2$$X$$_4$ ($A$ = Cd, Mg, $X$ = S, Se)

Our polycrystalline sample study on the Yb-based chalcogenide spinels $A$Yb$_2$$X_4$ ($A =$ Cd, Mg, $X =$ S, Se) has revealed frustrated magnetism due to the antiferromagnetically coupled Heisenberg spin on the pyrochlore lattice. Our crystal electric field analysis indicates the Yb ground state has nearly Heisenberg spins with a strong quantum character of the ground doublet. All the materials exhibit an antiferromagnetic order at 1.4-1.8 K, much lower temperature than the antiferromagnetic exchange coupling scale of $\sim 10$ K. The magnetic specific heat $C_{\rm M}$ shows a $T^{3}$ dependence, indicating the gapless feature in the Yb-based chalcogenide spinels. The magnetic entropy change much smaller than $R$ ln 2 below the Néel temperature and the small local magnetic field estimated from the $μ$SR measurements strongly suggest the significantly reduced size of the ordered moment in comparison with the bare moment size 1.33 $μ_{\rm B}$/Yb supporting strong fluctuations in the commensurate and incommensurate ordered states in CdYb$_2$S$_4$ and MgYb$_2$S$_4$, respectively.

cond-mat.str-el↗

arXiv2016

Magnetoelectric Behavior from $S=1/2$ Asymmetric Square Cupolas

Magnetoelectric properties are studied by a combined experimental and theoretical study of a quasi-two-dimensional material composed of square cupolas, Ba(TiO)Cu$_4$(PO$_4$)$_4$. The magnetization is measured up to above the saturation field, and several anomalies are observed depending on the field directions. We propose a $S$=1/2 spin model with Dzyaloshinskii-Moriya interactions, which well reproduces the full magnetization curves. Elaborating the phase diagram of the model, we show that the anomalies are explained by magnetoelectric phase transitions. Our theory also accounts for the scaling of the dielectric anomaly observed in experiments. The results elucidate the crucial role of the in-plane component of Dzyaloshinskii-Moriya interactions, which is induced by the noncoplanar buckling of square cupola. We also predict a `hidden' phase and another magnetoelectric response both of which appear in nonzero magnetic field.

cond-mat.str-el↗