arXiv subjects

Yusuke Tokunaga

Publications and source records attributed to Yusuke Tokunaga.

At least 19 recordsLinked to original sources

arXiv2026

Magnetoelastic mapping of the high-field phase diagram in the topological cubic helimagnet SrFeO$_{3}$

The cubic perovskite SrFeO$_{3}$ is a prototypical centrosymmetric itinerant magnet that hosts a quadruple-${\mathbf Q}$ hedgehog-antihedgehog lattice and exhibits a complex magnetic-field-temperature phase diagram. Yet, the microscopic mechanism underlying the emergence of its versatile multiple-${\mathbf Q}$ phases remains unresolved. Here, we reveal the field-orientation dependence of the magnetic phase diagram and establish an effective spin Hamiltonian for SrFeO$_{3}$ that incorporates a cubic single-ion anisotropy together with bilinear and biquadratic interactions in momentum space, which originate from the spin-charge coupling. In addition, we observe magnetoelastic signatures of a redistribution of the ligand-hole density upon entering the forced ferromagnetic phase. These findings emphasize the pivotal importance of electronic itinerancy arising from the formation of a ligand-hole band in stabilizing multiple-${\mathbf Q}$ phases.

cond-mat.str-el↗

arXiv2026

Magnetoelectric Control of Toroidal Moment in Ferroaxial Crystal PbMn$_{2}$Ni$_{6}$Te$_{3}$O$_{18}$

Ferroic multipole orders break some symmetry and often activate unique physical properties, such as nonreciprocal directional dichroism and linear magnetoelectric effects. Here, we demonstrate the control of magnetic toroidal orientation in PbMn$_{2}$Ni$_{6}$Te$_{3}$O$_{18}$ through the application of electric and magnetic fields in two distinct configurations. Through directional dichroism, we successfully visualize magnetic ferrotoroidic domains, establishing the intrinsic coupling among magnetic toroidal moment, crystallographic ferroaxial moment, and magnetoelectric monopoles. Our findings not only present an effective pathway for controlling magnetic toroidal moment but also provide a novel approach for investigating ferroaxial ordering.

cond-mat.str-el↗

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

Effect of uniaxial stress on helimagnetic phases in the square-lattice itinerant magnet EuAl$_{4}$

We investigate uniaxial-stress effects on the magnetic phase diagram of the square-lattice itinerant magnet EuAl$_{4}$, where strong coupling among spin, lattice, and charge produces a variety of helimagnetic phases, including rhombic and square skyrmion lattices. Combining resistivity and magnetization measurements with neutron scattering, we find that compressive stresses of only several tens of megapascal along [010] enhance antiferromagnetic character and shorten the magnetic modulation period in the lowest-temperature single-Q spiral state, thereby driving the critical temperatures and fields of multiple phases to higher values. First-principles calculations show that increasing orthorhombic lattice distortion deforms the Fermi surface relevant to the magnetism, providing compelling evidence that Fermi-surface nesting plays a crucial role in stabilizing the helical magnetic modulations in EuAl$_{4}$.

cond-mat.str-el↗

arXiv2025

Linear tetramer formation in nonmagnetic pyrochlore niobate

We investigate displacive short-range order in pyrochlore Y2Nb2O7, which exhibits a nonmagnetic insulating state despite the presence of formally tetravalent Nb4+ (S = 1/2) ions on the pyrochlore network. Synchrotron x-ray diffraction on a single crystal reveals a characteristic x-ray diffuse scattering (XDS) pattern primarily around q = {0.5, 0.5, 2}. Reverse Monte Carlo (RMC) simulations uncover local Nb displacements along the <111> axes, leading to the formation of linear Nb4 tetramers. Our findings highlight a crucial role of molecular orbital degrees of freedom in stabilizing the nonmagnetic insulating state. This study demonstrates that RMC analysis of XDS provides a powerful approach for elucidating short-range correlations and the underlying mechanisms governing the physical properties of crystalline materials.

cond-mat.str-el↗

arXiv2025

All-optical control of antiferromagnetic domains via an inverse optical magnetoelectric effect

Antiferromagnets are a promising platform for next-generation spintronics due to their ultrafast spin dynamics and robustness to external fields. All-optical control of antiferromagnetic order is essential to fully exploit their potential in energy-efficient and high-speed spintronic and memory applications. However, optical writing of antiferromagnetic domains remains a fundamental challenge, as conventional magneto-optical techniques rely on net magnetization, which is absent in antiferromagnets. In certain multiferroic antiferromagnets, the magnetic toroidal moment provides an additional degree of freedom through its inherent magnetoelectric coupling. This coupling at higher frequencies results in the optical magnetoelectric effect (OME), which manifests as a directional asymmetry in light propagation and enables optical probing of antiferromagnetic states. Here, we demonstrate all-optical writing of antiferromagnetic domains using the inverse optical magnetoelectric effect (IOME) in ferrotoroidic LiNiPO4. The writing process is nonvolatile, non-thermal, and deterministic, driven solely by reversing the light propagation direction. This directional control arises from a strong coupling between the photon linear momentum and the magnetic toroidal moment, enabling the repeatable switching between time-reversed domains with arbitrary light polarization. Our findings establish IOME as a distinct mechanism for manipulating antiferromagnetic order, opening a new paradigm in opto-magnetism driven by photon momentum.

cond-mat.mtrl-sci↗

arXiv2025

Distribution of antiferromagnetic rare-earth domains in multiferroic Dy$_{0.7}$Tb$_{0.3}$FeO$_3$

In many multiferroics, rare-earth and transition-metal orders exist side by side. For analyzing their interaction and its consequences for the multiferroic state, the associated domain patterns and their spatial correlation can give valuable insight. Unfortunately, this is often hampered by the lack of access to the domains of the rare-earth order. Here, we uncover such a domain pattern for the antiferromagnetic and multiferroic Dy$_{0.7}$Tb$_{0.3}$FeO$_3$. Optical second harmonic generation reveals the formation of column-like Dy/Tb domains. Interestingly, the columns form perpendicular to the magnetically induced electric polarization. Hence, the antiferromagnetic rare-earth order forces the ferroelectric domains to form nominally charged head-to-head and tail-to-tail domain walls, thus playing a leading role in the domain formation within the multiferroic phase. In turn, to reduce energy cost, the ferroelectric order causes a reduced rare-earth domain-wall density along the direction of the electric polarization. This interplay highlights the multiferroic character of the Dy$_{0.7}$Tb$_{0.3}$FeO$_3$ domain pattern. We position Dy$_{0.7}$Tb$_{0.3}$FeO$_3$ within the broader landscape of rare-earth multiferroics and identify three distinct scenarios for the role of rare-earth order in these.

cond-mat.mtrl-sci↗

arXiv2025

Piezoelectric Transition in a Nonpyroelectric Gyroidal Metal-Organic Framework

Among the thirty-two crystallographic point groups, 432 is the only one that lacks an inversion center but does not exhibit piezoelectricity. A gyroidal structure belongs to point group 432 and shows characteristic physical properties attributed to its distinctive strong isotropic network. Here, we investigate a gyroidal cobalt oxalate metal-organic framework (MOF) with disordered orientations of SO4 tetrahedra. Synchrotron X-ray diffraction experiments using a single crystal reveal a cubic-to-cubic structural phase transition at TS = 120 K. This transition involves a change in the point group from nonpiezoelectric 432 to piezoelectric 23. The symmetry change arises from the ordering of distorted SO4 molecules, leading to a three-dimensional helical arrangement of electric dipole moments. Furthermore, pyroelectric current measurements using polycrystalline pellet samples reveal that electric polarization emerges below TS depending on the magnitude of the pelletizing pressure, demonstrating piezoelectricity. The gyroidal MOF offers an opportunity to explore unique dielectric properties induced by the helical ordering of molecules and structural flexibility.

cond-mat.mtrl-sci↗

arXiv2024

Contrasting magnetothermal conductivity in sibling Co-based honeycomb-lattice antiferromagnets

Honeycomb-lattice antiferromagnets have attracted wide attention for exploration of exotic heat transport and their interplay with magnetic excitations. In this work, we have revealed a contrasting behavior in the magneto-thermal conductivity (MTC) between two Co-based honeycomb-lattice magnets Co4M2O9 (M = Nb, Ta), despite their identical lattice structures and quite similar magnetism. Co4Ta2O9 exhibits enhanced MTC of about 550% at 9 T of an in-plane magnetic field, comparable to other honeycomb-magnets, while MTC for Co4Nb2O9 reaches only ~30%. This marked difference is ascribed to distinct features in the field-induced evolution of magnetic excitations that resonantly scatter phonons. This finding sheds light on implicit impacts of non-magnetic ions on thermal transport, and hints at the potential for broad heat-transport tunability while preserving magnetism and lattice structures.

cond-mat.str-el↗

arXiv2024

Spin-lattice-coupled helical magnetic order in breathing pyrochlore magnets, CuAlCr$_{4}$S$_{8}$ and CuGaCr$_{4}$S$_{8}$

We report low-temperature powder X-ray and neutron diffraction studies on breathing pyrochlore magnets Cu$M$Cr$_{4}$S$_{8}$ ($M$ = Al, Ga), which undergo a magnetic transition at $T_{\rm N} \approx$ 21 and 31 K for {$M$ = Al and Ga, respectively. X-ray diffraction reveals that the magnetic transition accompanies a structural transition from cubic $F{\overline 4}3m$ to polar orthorhombic $Imm2$ symmetry for both the compounds, with larger distortion observed for $M$ = Ga at low temperatures. Neutron diffraction reveals incommensurate magnetic modulation ${\mathbf Q} = (q_{\rm IC}, 0.5, 0)$ in the orthorhombic setting, where $q_{\rm IC} \approx$ 0.39 and 0.31 for $M$ = Al and Ga, respectively. Our magnetic-structure analysis suggests cycloid-type magnetic order but not proper-screw type for both the compounds. We find strong correlation between the local spin configuration and Cr-Cr bond lengths, indicating that the spin-lattice coupling as well as the magnetic frustration play an important role in determining the ground state. Cu$M$Cr$_{4}$S$_{8}$ potentially offers a platform to explore magnetoelectric effects arising from the helimagnet driven electric polarity.

cond-mat.mtrl-sci↗

arXiv2024

Cluster rearrangement by chiral charge order in lacunar spinel GaNb$_4$Se$_8$

Transition-metal atoms with d electrons sometimes form clusters in crystals, which significantly affects the physical properties. Such a cluster formation frequently accompanies a change in the crystal system, leading to the presence of domains with different crystal orientations. In particular, the cubic symmetry is rarely retained after the cluster formation. Here, we identify a cubic-to-cubic phase transition in lacunar spinel GaNb$_4$Se$_8$, where the change in the lattice parameter is less than 0.0001%. Each Nb$^{3.25+}$ tetramer with seven 4d electrons is distorted into a Nb$^{3+}$ trimer and a Nb$^{4+}$ monomer induced by charge disproportionation among Nb ions. While the Nb$^{3+}$ trimer with six 4d electrons forms spin-singlets in the sigma-bonding orbitals for three Nb-Nb bonds, a localized S=1/2 spin remains on the Nb$^{4+}$ ion. Furthermore, a local electric dipole moment is induced along the three-fold rotation axis of each distorted tetramer by the cluster rearrangement. The electric dipole moments are regularly arranged to maintain the cubic symmetry, giving rise to chiral order.

cond-mat.str-el↗

arXiv2023

Real-Space Observation of Ligand Hole State in Cubic Perovskite SrFeO$_3$

An anomalously high valence state sometimes shows up in transition-metal oxide compounds. In such systems, holes tend to occupy mainly the ligand $p$ orbitals, giving rise to interesting physical properties such as superconductivity in cuprates and rich magnetic phases in ferrates. However, no one has ever observed the distribution of ligand holes in real space. Here, we report a successful observation of the spatial distribution of valence electrons in cubic perovskite SrFeO$_3$ by high-energy X-ray diffraction experiments and precise electron density analysis using a core differential Fourier synthesis method. A real-space picture of ligand holes formed by the orbital hybridization of Fe 3$d$ and O 2$p$ is revealed. The anomalous valence state in Fe is attributed to the considerable contribution of the ligand hole, which is related to the metallic nature and the absence of Jahn-Teller distortions in this system.

cond-mat.str-el↗

arXiv2023

Magnetoelectrocaloric effect of multiferroic GdFeO3

We report an experimental demonstration of the magnetoelectrocaloric effect (MECE) in multiferroic $\mathrm{GdFeO_3}$. The temperature of the magnetic material changes when an external electric field is suddenly changed. MECE is the largest below the ordering temperature of Gd moments and modifiable by a magnetic field, suggesting that the ferroelectric transition affects MECE. The observed MECE shows a higher energy efficiency than typical magnetocaloric effects and adiabatic nuclear demagnetization. The present findings provide a proof of concept of MECE in multiferroics.

cond-mat.str-el↗

arXiv2023

Spin-lattice and magnetoelectric couplings enhanced by orbital degrees of freedom in polar magnets

Orbital degrees of freedom mediating an interaction between spin and lattice were predicted to raise strong magnetoelectric effect, i.e. realize an efficient coupling between magnetic and ferroelectric orders. However, the effect of orbital fluctuations have been considered only in a few magnetoelectric materials, as orbital degeneracy driven Jahn-Teller effect rarely couples to polarization. Here, we explore the spin-lattice coupling in multiferroic Swedenborgites with mixed valence and Jahn-Teller active transition metal ions on a stacked triangular/Kagome lattice using infrared and dielectric spectroscopy. On one hand, in CaBa$M_4$O$_7$ ($M$ = Co, Fe), we observe strong magnetic order induced shift in the phonon frequencies and a corresponding large change in the dielectric response. Remarkably, as an unusual manifestation of the spin-phonon coupling, the spin-fluctuations reduce the phonon life-time by an order of magnitude at the magnetic phase transitions. On the other hand, lattice vibrations, dielectric response, and electric polarization show no variation at the Néel temperature of CaBaFe$_2$Co$_2$O$_7$, which is built up by orbital singlet ions. Our results provide a showcase for orbital degrees of freedom enhanced magnetoelectric coupling via the example of Swedenborgites.

cond-mat.str-el↗

arXiv2022

Topological Thermal Hall Effect of Magnons in Magnetic Skyrmion Lattice

Topological transports of fermions are governed by the Chern numbers of the energy bands lying below the Fermi energy. For bosons, e.g. phonons and magnons in a crystal, topological transport is dominated by the Chern number of the lowest energy band when the band gap is comparable to the thermal energy. Here, we demonstrate the presence of topological transport by bosonic magnons in a lattice of magnetic skyrmions - topological defects formed by a vortex-like texture of spins. We find a distinct thermal Hall signal in the magnetic skyrmion phase of an insulating polar magnet GaV4Se8, identified as the topological thermal Hall effect of magnons governed by the Chern number of the lowest energy band of the magnons in a triangular lattice of magnetic skyrmions. Our findings lay a foundation for studying topological phenomena of other bosonic excitations through thermal Hall probe.

cond-mat.str-el↗

arXiv2021

Switching of antiferromagnetic states in LiCoPO$_4$ as investigated via the magnetoelectric effect

The linear magnetoelectric (ME) effect allows for the selection or switching between two antiferromagnetic (AFM) states via the application of large electric ($E$) and magnetic ($H$) fields. Once an AFM state is selected, it is preserved by an energy barrier, even when the fields are removed. Using a simple phenomenological model, we find that this energy barrier, needed to switch the AFM state, is proportional to the product of the $E$ and $H$ coercive fields $(EH)_{\rm C}$. We measured the field and temperature dependence of $(EH)_{\rm C}$ in LiCoPO$_4$ for two different field configurations, and the data show the temperature variation of $(EH)_{\rm C}\sim(T_{\rm N}-T)^{3/2}$ in good agreement with the model. We also investigated the dynamics of the AFM domain switching using pulsed $E$-field measurements. It was found that the coercive field $(EH)_{\rm C}$ follows a power-law frequency dependence and is well described in the framework of Ishibashi-Orihara model, implying 1-dimensional character of domain wall propagation.

cond-mat.str-el↗

arXiv2021

Magnetoelectric spectroscopy of spin excitations in LiCoPO4

We have studied spin excitations in a single-domain crystal of antiferromagnetic LiCoPO4 by THz absorption spectroscopy. By analyzing the selection rules and comparing the strengths of the absorption peaks in the different antiferromagnetic domains, we found electromagnons and magnetoelectric spin resonances besides conventional magnetic-dipole active spin-wave excitations. Using the sum rule for the magnetoelectric susceptibility we determined the contribution of the spin excitations to all the different off-diagonal elements of the static magnetoelectric susceptibility tensor in zero as well as in finite magnetic fields. We conclude that the magnetoelectric spin resonances are responsible for the static magnetoelectric response of the bulk when the magnetic field is along the x-axis, and the symmetric part of the magnetoelectric tensor with zero diagonal elements dominates over the antisymmetric components.

cond-mat.str-el↗

arXiv2019

Metamagnetic transitions and magnetoelectric responses in a chiral polar helimagnet Ni$_2$InSbO$_6$

Magnetic-field effect on the magnetic and electric properties in a chiral polar ordered corundum Ni$_2$InSbO$_6$ has been investigated. Single-crystal soft x-ray and neutron diffraction measurements confirm long-wavelength magnetic modulation. The modulation direction tends to align along the magnetic field applied perpendicular to the polar axis, suggesting that the nearly proper-screw type helicoid should be formed below 77\,K. The application of a high magnetic field causes a metamagnetic transition. In a magnetic field applied perpendicular to the polar axis, a helix-to-canted antiferromagnetic transition takes place through the intermediate soliton lattice type state. On the other hand, a magnetic field applied along the polar axis induces a first-order metamagnetic transition. These metamagnetic transitions accompany a change in the electric polarization along the polar axis.

cond-mat.mtrl-sci↗