arXiv subjects

Hiroshi Kageyama

Publications and source records attributed to Hiroshi Kageyama.

At least 19 recordsLinked to original sources

arXiv2026

Pinwheel-shaped bound triplet pairs in the magnetization plateaus of SrCu$_2$(BO$_3$)$_2$

The sequence of magnetization plateaus at 1/8, 2/15, 1/6, 1/4, 1/3, 2/5, and 1/2 of the saturation observed in SrCu$_2$(BO$_3$)$_2$ remained a puzzle until tensor-networks-based numerical simulations suggested that the low-magnetization plateaus are stabilized as Wigner crystals of spin-2 bound states, and not as one of the standard configurations (semiclassical up-down, or crystals of triplets). We report on $^{63,65}$Cu nuclear magnetic resonance spectra up to 41.9 T: Based on constraints deduced from the 1/3 plateau, we show that the spectra in the 1/8 and 2/15 plateaus indeed agree with the prediction for the spin-2 bound states, while being incompatible with a crystal of triplets. This adds the formation of Wigner crystals of bound states as an alternative fundamental paradigm in the theory of magnetization plateaus.

cond-mat.str-el↗

arXiv2025

Design and theory of switchable linear magnetoelectricity by ferroelectricity in Type-I multiferroics

We present a comprehensive theoretical investigation of magnetoelectric (ME) coupling mechanisms in 19 altermagnetic and 4 ferrimagnetic Type-I multiferroics using electronic band structure calculations with spin-orbit coupling, a first-principles ME response framework, and spin-space-group theory analysis. We formulate a universal scheme for realizing nonvolatile ME coupling in Type-I multiferroics, where two distinct pathways emerge, each dictated by spin-space symmetry. The first pathway is associated with switching of the spin splitting or the now familiar spin-momentum locking in reciprocal space, characteristic of some altermagnetic mul-tiferroics that exhibit coexisting antiferromagnetism and ferroelectricity. The second pathway involves real-space magnetization switching via electric polarization reversal, characterized by switchable components of the linear ME tensor, despite the traditionally weak coupling in Type-I systems due to the independent origins of magnetism and ferroelectricity. We demonstrate that these two intrinsic ME coupling mechanisms are mutually exclusive and propose thermodynami-cally stable compounds for experimentation. Our findings establish general design principles for controlling robust nonvolatile ME effects in multiferroic materials.

cond-mat.mtrl-sci↗

arXiv2025

Miniaturized and robust tunable monochromatic magneto-optical platform for pulsed magnetic fields

Tunable monochromatic magneto-transmission is one of the most established magneto-optical techniques, particularly well suited for pulsed magnetic fields. It employs fixed-wavelength monochromatic light as the probe, while the magnetic field is swept to bring the sample into resonance with the photon energy. The key component of this setup is a tunable laser system, typically consisting of a Ti:sapphire laser coupled with an optical parametric oscillator. However, such laser systems are often bulky, expensive, and inherently unstable, which significantly limits their widespread application in magneto-optical laboratories. In this work, we develop a high-accuracy, cost-effective, and compact tunable monochromatic magneto-transmission system based on a combination of a laser-driven white light source and a mini monochromator, and demonstrate its feasibility and performance in a millisecond-range pulsed magnetic field condition. To verify the accuracy of this new and simplified setup, we performed Faraday rotation measurements on the geometrically frustrated spin system CdCr2O4, as well as magneto-transmission experiments on the Shastry-Sutherland lattice antiferromagnet SrCu2(BO3)2. These results show excellent agreement with previous reports, confirming the reliability and precision of the new setup.

cond-mat.str-el↗

arXiv2023

Superconductivity in Ternary Germanide ScPdGe and Silicide ScPdSi

The electronic properties of ScPdGe and ScPdSi, crystallizing in the hexagonal ZrNiAl and orthorhombic TiNiSi structures, respectively, are investigated. ScPdGe and ScPdSi are found to show bulk superconductivity below 0.9 and 1.7 K, respectively, based on electrical resistivity and heat capacity data measured using synthesized polycrystalline samples. First principles calculations indicate the presence of large contributions of Sc 3d and Pd 4d electrons at the Fermi energy in both materials. The electronic properties and electronic states of these materials are discussed in comparison with those of several superconductors containing scandium and a 4d transition metal element.

cond-mat.supr-con↗

arXiv2023

Thermal Magnetoelectrics in all Inorganic Quasi-Two-Dimensional Halide Perovskites

From lithium-ion batteries to high-temperature superconductors, oxide materials have been widely used in electronic devices. However, demands of future technologies require materials beyond oxides, as anion chemistries distinct from oxygen can expand the palette of mechanisms and phenomena, to achieve superior functionalities. Examples include nitride-based wide bandgap semiconductors and halide perovskite solar cells, with MAPbBr3 being a representation revolutionizing photovoltaics research. Here, we demonstrate magnetoelectric behaviour in quasi-two-dimensional halides (K,Rb)3Mn2Cl7 through simultaneous thermal control of electric and magnetic polarizations by exploiting a polar-to-antipolar displacive transition. Additionally, our calculations indicate a possible polarization switching path including a strong magnetoelectric coupling, indicating halides can be excellent platforms to design future multiferroic and ferroelectric devices. We expect our findings to broaden the exploration of multiferroics to non-oxide materials and open access to novel mechanisms, beyond conventional electric/magnetic control, for coupling ferroic orders.

cond-mat.mtrl-sci↗

arXiv2023

Field-induced bound-state condensation and spin-nematic phase in SrCu$_2$(BO$_3$)$_2$ revealed by neutron scattering up to 25.9 T

Bose-Einstein condensation (BEC) underpins exotic forms of order ranging from superconductivity to superfluid 4 He. In quantum magnetic materials, ordered phases induced by an applied magnetic field can be described as the BEC of magnon excitations. With sufficiently strong magnetic frustration, exemplified by the system SrCu$_2$(BO$_3$)$_2$ , no clear magnon BEC is observed and the complex spectrum of multi-magnon bound states may allow a different type of condensation, but the high fields required to probe this physics have remained a barrier to detailed investigation. Here we exploit the first purpose-built high-field neutron scattering facility to measure the spin excitations of SrCu$_2$(BO$_3$)$_2$ up to 25.9 T and use cylinder matrix-product-states (MPS) calculations to reproduce the experimental spectra with high accuracy. Multiple unconventional features point to a condensation of $S = 2$ bound states into a spin-nematic phase, including the gradients of the one-magnon branches, the presence of many novel composite two- and three-triplon excitations and the persistence of a one-magnon spin gap. This gap reflects a direct analogy with superconductivity, suggesting that the spin-nematic phase in SrCu$_2$(BO$_3$)$_2$ is best understood as a condensate of bosonic Cooper pairs. Our results underline the wealth of unconventional states yet to be found in frustrated quantum magnetic materials under extreme conditions.

cond-mat.str-el↗

arXiv2023

Generation of third-harmonic spin oscillation from strong spin precession induced by terahertz magnetic near fields

The ability to drive a spin system to state far from the equilibrium is indispensable for investigating spin structures of antiferromagnets and their functional nonlinearities for spintronics. While optical methods have been considered for spin excitation, terahertz (THz) pulses appear to be a more convenient means of direct spin excitation without requiring coupling between spins and orbitals or phonons. However, room-temperature responses are usually limited to small deviations from the equilibrium state because of the relatively weak THz magnetic fields in common approaches. Here, we studied the magnetization dynamics in a HoFeO3 crystal at room temperature. A custom-made spiral-shaped microstructure was used to locally generate a strong multicycle THz magnetic near field perpendicular to the crystal surface; the maximum magnetic field amplitude of about 2 T was achieved. The observed time-resolved change in the Faraday ellipticity clearly showed second- and third-order harmonics of the magnetization oscillation and an asymmetric oscillation behaviour. Not only the ferromagnetic vector M but also the antiferromagnetic vector L plays an important role in the nonlinear dynamics of spin systems far from equilibrium.

physics.optics↗

arXiv2023

Simultaneous measurement of specific heat and thermal conductivity in pulsed magnetic fields

We report an experimental setup for simultaneously measuring specific heat and thermal conductivity in feedback-controlled pulsed magnetic fields of 50 msec duration at cryogenic temperatures. A stabilized magnetic field pulse obtained by the feedback control, which dramatically improves the thermal stability of the setup and sample, is used in combination with the flash method to obtain absolute values of thermal properties up to 37.2 T in the 2 K to 16 K temperature range. We describe the experimental setup and demonstrate the performance of the present method with measurements on single crystal samples of the geometrically frustrated quantum spin-dimer system SrCu$_2$(BO$_3$)$_2$. Our proof-of-principle results show excellent agreement with data taken using a standard steady-state method, confirming the validity and convenience of the present approach.

cond-mat.str-el↗

arXiv2022

Honeycomb Layered Oxides With Silver Atom Bilayers and Emergence of Non-Abelian SU(2) Interactions

Honeycomb layered oxides with monovalent or divalent, monolayered cationic lattices generally exhibit myriad crystalline features encompassing rich electrochemistry, geometries and disorders, which particularly places them as attractive material candidates for next-generation energy storage applications. Herein, we report global honeycomb layered oxide compositions, ${\rm Ag_2}M_2{\rm TeO_6}$ ($M = \rm Ni, Mg, \textit{etc}.$) exhibiting $\rm Ag$ atom bilayers with sub-valent states within Ag-rich crystalline domains of ${\rm Ag_6}M_2{\rm TeO_6}$ and $\rm Ag$-deficient domains of ${\rm Ag}_{2 - x}\rm Ni_2TeO_6$ ($0 < x < 2$). The $\rm Ag$-rich material characterised by aberration-corrected transmission electron microscopy reveals local atomic structural disorders characterised by aperiodic stacking and incoherency in the bilayer arrangement of $\rm Ag$ atoms. Meanwhile, the global material not only displays high ionic conductivity, but also manifests oxygen-hole electrochemistry during silver-ion extraction. Within the $\rm Ag$-rich domains, the bilayered structure, argentophilic interactions therein and the expected $\rm Ag$ sub-valent states ($1/2+, 2/3+, \textit{etc}.$) are theoretically understood via spontaneous symmetry breaking of SU($2$)$\times$U($1$) gauge symmetry interactions amongst $3$ degenerate mass-less chiral fermion states, justified by electron occupancy of silver $4d_{z^2}$ and $5s$ orbitals on a bifurcated honeycomb lattice. This implies that bilayered frameworks have research applications that go beyond the confines of energy storage.

cond-mat.mtrl-sci↗

arXiv2022

Magnetically hidden state on the ground floor of the magnetic Devil's staircase

We investigated the low-temperature and high-field thermodynamic and ultrasonic properties of SrCu2(BO3)2, which exhibits various plateaux in its magnetization curve above 27~T, called a magnetic Devil's staircase. The results of the present study confirm that magnetic crystallization, the first step of the staircase, occurs above 27~T as a 1st-order transition accompanied by a sharp singularity in heat capacity $C_p$ and a kink in the elastic constant. In addition, we observe a thermodynamic anomaly at lower fields around 26~T, which has not been previously detected by any magnetic probes. At low temperatures, this magnetically hidden state has a large entropy and does not exhibit Schottky-type gapped behavior, which suggests the existence of low-energy collective excitations. Based on our observations and theoretical predictions, we propose that magnetic quadrupoles form a spin-nematic state around 26~T as a hidden state on the ground floor of the magnetic Devil's staircase.

cond-mat.str-el↗

arXiv2021

Thermally populated versus field-induced triplon bound states in the Shastry-Sutherland lattice SrCu$_2$(BO$_3$)$_2$

The Shastry-Sutherland compound SrCu$_2$(BO$_3$)$_2$ constituting orthogonally coupled dimers harbors a $S=0$ singlet ground state. The confluence of strong interdimer interaction and frustration engenders a spectrum of low-energy excitations including localized triplons as well as singlet and triplet bound states. Their dynamics are controlled by an external magnetic field and temperature. Here, we employ high-field Raman spectroscopy to map the field and temperature evolution of such bosonic composite quasiparticles on approaching the 1/8 magnetization plateau. Our study unveils that the magnetic field and thermal fluctuations show remarkably similar effects in melting the singlet bound states, but are disparate in their effects on the fine spectral shapes. This, together with the anti-crossing of two singlet bound states in the intermediate field $B=10-16$ T, is discussed in terms of the correlated dynamics of frustrated, interacting bosons.

cond-mat.str-el↗

arXiv2021

Uniform structural phase transition in V$_2$O$_3$ without short-range distortions of the local structure

The local structure of V$_{2}$O$_{3}$, an archetypal strongly correlated electron system that displays a metal-insulator transition around 160 K, has been investigated via pair distribution function (PDF) analysis of neutron and x-ray total scattering data. The rhombohedral-to-monoclinic structural phase transition manifests as an abrupt change on all length scales in the observed PDF. No monoclinic distortions of the local structure are found above the transition, although coexisting regions of phase-separated rhombohedral and monoclinic symmetry are observed between 150 K and 160 K. This lack of structural fluctuations above the transition contrasts with the known presence of magnetic fluctuations in the high-temperature state, suggesting that the lattice degree of freedom plays a secondary role behind the spin degree of freedom in the transition mechanism.

cond-mat.str-el↗

arXiv2021

Mixed Alkali-Ion Transport and Storage in Atomic-Disordered Honeycomb Layered $\rm NaKNi_2TeO_6$

Honeycomb layered oxides constitute an emerging class of materials that show interesting physicochemical and electrochemical properties. However, the development of these materials is still limited. Here, we report the combined use of alkali atoms ($\rm Na$ and $\rm K$) to produce a mixed alkali honeycomb layered oxide material, namely, $\rm NaKNi_2TeO_6$. Via transmission electron microscopy measurements, we reveal the local atomic structural disorders characterised by aperiodic stacking and incoherency in the alternating arrangement of $\rm Na$ and $\rm K$ atoms. We also investigate the possibility of mixed electrochemical transport and storage of $\rm Na$ and $\rm K$ ions in $\rm NaKNi_2TeO_6$. In particular, we report an average discharge cell voltage of about $4\, \rm V$ and a specific capacity of around $80\, \rm mAh\, g^{-1}$ at low specific currents (i.e., $< 10\, \rm mA\, g^{-1}$) when a $\rm NaKNi_2TeO_6$-based positive electrode is combined with a room-temperature $\rm NaK$ liquid alloy negative electrode using an ionic liquid-based electrolyte solution. These results represent a step towards the use of tailored cathode active materials for dendrite-free electrochemical energy storage systems exploiting room-temperature liquid alkali metal alloy materials.

cond-mat.mtrl-sci↗

arXiv2021

Superconductivity in Nb2Pd3Te5 and Chemically-Doped Ta2Pd3Te5

We report on the superconductivity in ternary transition metal tellurides Ta2Pd3Te5 and Nb2Pd3Te5, which have a one-dimensional crystal structure. Single-crystalline and polycrystalline samples of Ta2Pd3Te5 show nonmetallic electron conduction, while Ti or W doping results in metallic behavior with a bulk superconducting transition at 2-4 K. In contrast, the polycrystalline samples of Nb2Pd3Te5, which are found to be isostructural to Ta2Pd3Te5, show a bulk superconducting transition at 3.3 K. The crystal structure and physical properties of Ta2Pd3Te5 and Nb2Pd3Te5 are also discussed in comparison with a candidate excitonic insulator Ta2NiSe5.

cond-mat.supr-con↗

arXiv2020

Molecular beam epitaxy growth of the highly conductive oxide SrMoO$_3$

SrMoO$_3$ is a promising material for its excellent electrical conductivity, but growing high-quality thin films remains a challenge. Here we synthesized epitaxial films of SrMoO$_3$ using the molecular beam epitaxy (MBE) technique under a low oxygen-flow rate. Introduction of SrTiO$_3$ buffer layers of 4--8 unit cells between the film and the (001)-oriented SrTiO$_3$ or KTaO$_3$ substrate was crucial to remove impurities and/or roughness of the film surface. The obtained film shows improved electrical conductivities as compared with films obtained by other techniques. The high quality of the SrMoO$_3$ film is also verified by angle-resolved photoemission spectroscopy (ARPES) measurements showing clear Fermi surfaces.

cond-mat.mtrl-sci↗

arXiv2020

Epitaxial stabilization of SrCu$_3$O$_4$ with infinite Cu$_{3/2}$O$_2$ layers

We report the epitaxial thin film synthesis of SrCu$_3$O$_4$ with infinitely stacked Cu$_3$O$_4$ layers composed of edge-sharing CuO$_4$ square-planes, using molecular beam epitaxy. Experimental and theoretical characterizations showed that this material is a metastable phase that can exist by applying tensile biaxial strain from the (001)-SrTiO$_3$ substrate. SrCu$_3$O$_4$ shows an insulating electrical resistivity in accordance with the Cu$^{2+}$ valence state revealed X-ray photoelectron spectroscopy. First-principles calculations also indicated that the unoccupied $d_{3z^2-r^2}$ band becomes substantially stabilized owing to the absence of apical anions, in contrast to $A_2$Cu$_3$O$_4$Cl$_2$ ($A = $Sr, Ba) with an $A_2$Cl$_2$ block layer and therefore a trans-CuO$_4$Cl$_2$ octahedron. These results suggest that SrCu$_3$O$_4$ is a suitable parent material for electron-doped superconductivity based on the Cu$_3$O$_4$ plane.

cond-mat.mtrl-sci↗

arXiv2020

Hidden Ladder in SrMoO$_3$/SrTiO$_3$ Superlattices: Experiments and Theoretical Calculations

A double-layered perovskite oxide Sr$_3$Mo$_2$O$_7$ is considered a "hidden ladder" system with wide and narrow bands near the Fermi level, for which high-$T_{\rm c}$ superconductivity is expected. However, the difficulty in synthesis, especially in the preparation of samples without oxygen deficiency, can hinder the observation of superconductivity. In this study, we constructed a double-layer SrMoO$_3$ block through artificial superlattices with the insulating SrTiO$_3$ block, (SrMoO$_3$)$_m$/(SrTiO$_3$)$_t$ ($m = 2, 4$; $t = 4$). First-principles calculations for bilayered SrMoO$_3$ ($m = 2$) exhibit a wide-narrow band structure near the Fermi level, which bears a close resemblance to Sr$_3$Mo$_2$O$_7$. The dispersion along the $k_z$ direction is strongly suppressed by increasing the number of the SrTiO$_3$ layers, $t$. However, no superconductivity is observed down to 0.1 K. We discuss the absence of the superconductivity for the present films on the basis of results of scanning transmission electron microscopy and band structure calculations.

cond-mat.str-el↗

arXiv2020

High-Mobility Carriers Induced by Chemical Doping in the Candidate Nodal-Line Semimetal CaAgP

We report the electronic properties of single crystals of candidate nodal-line semimetal CaAgP. The transport properties of CaAgP are understood within the framework of a hole-doped nodal-line semimetal. In contrast, Pd-doped CaAgP shows a drastic increase of magnetoresistance at low magnetic fields and a strong decrease of electrical resistivity at low temperatures probably due to weak antilocalization. Hall conductivity data indicated that the Pd-doped CaAgP has not only hole carriers induced by the Pd doping, but also high-mobility electron carriers in proximity of the Dirac point. Electrical resistivity of Pd-doped CaAgP also showed a superconducting transition with onset temperature of 1.7-1.8 K.

cond-mat.mtrl-sci↗