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Shinichiro Asai

Publications and source records attributed to Shinichiro Asai.

At least 19 recordsLinked to original sources

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

Observation of Altermagnetic Order Switching in Bulk MnTe by Polarized Neutron Diffraction

Altermagnetic order, characterized by the Néel vector, breaks time-reversal symmetry (TRS) even in the nonrelativistic limit. Although spin-polarized and anomalous transport phenomena emerge with this order, they are mutually compensated by TRS-connected antiphase domains with opposite Néel vectors. Here we employ polarized neutron diffraction to directly probe the altermagnetic order in MnTe. Pronounced nuclear-magnetic interference terms were observed, providing direct evidence of a net Néel vector in the bulk crystal. Moreover, a weak ferromagnetic moment (WFM), originating from relativistic spin-orbit coupling, was found to be coupled with the altermagnetic order. Both the altermagnetic order and the WFM can be switched by milli-Tesla-scale magnetic field cooling.

cond-mat.str-el

Observation of Switchable Chiral Magnons in an Altermagnet

Chiral magnons, the quanta of handed spin waves, transport spin angular momentum without energy loss due to Joule heating. The recently discovered altermagnets were proposed to host chiral magnons arising from a non-relativistic exchange mechanism, similar to that in ferromagnets but without net magnetization, offering a stray-field-free platform for efficient magnon spin-current manipulation. In this work, we directly observed chiral magnons in the altermagnetic prototype MnTe using polarized inelastic neutron scattering. Furthermore, the magnon chirality was found to be reversibly switched by magnetic-field control, establishing a robust foundation for functional altermagnetic magnonics.

cond-mat.str-el

Kitaev interaction and proximate higher-order skyrmion crystal in the triangular lattice van der Waals antiferromagnet NiI2

Topological spin textures, such as magnetic skyrmions, are a spectacular manifestation of magnetic frustration and anisotropy. Most known skyrmion systems are restricted to a topological charge of one, require an external magnetic field for stabilization, and are only reported in a few materials. Here, we investigate the possibility that the Kitaev anisotropic-exchange interaction stabilizes a higher-order skyrmion crystal in the insulating van der Waals magnet NiI2. We unveil and explain the incommensurate static and dynamic magnetic correlations across three temperature-driven magnetic phases of this compound using neutron scattering measurements, simulations, and modeling. Our parameter optimisation yields a minimal Kitaev-Heisenberg Hamiltonian for NiI2 which reproduces the experimentally observed magnetic excitations. Monte Carlo simulations for this model predict the emergence of the higher-order skyrmion crystal but neutron diffraction and optical experiments in the candidate intermediate temperature regime are inconclusive. We discuss possible deviations from the Kitaev-Heisenberg model that explains our results and conclude that NiI2, in addition to multiferroic properties in the bulk and few-layer limits, is a Kitaev bulk material proximate to the finite temperature higher-order skyrmion crystal phase.

cond-mat.mtrl-sci

Dirac Magnon in Honeycomb Lattice Magnet NiTiO3

We performed inelastic neutron scattering experiments on single-crystal samples of the honeycomb lattice magnet, ilmenite NiTiO3. Below the Neel temperature of 22 K, spin wave excitations with a band energy of 3.7 meV were observed. The neutron energy spectra were well-reproduced by modeling the system as a ferromagnetic honeycomb lattice with antiferromagnetic interlayer coupling, using linear spin wave theory. Similar to another ilmenite CoTiO3, a crossing structure was observed at the K point, suggesting the resence of Dirac magnons in NiTiO3. Further calculations suggested the formation of Dirac nodal line.

cond-mat.str-el

Unusual spin dynamics in the van der Waals antiferromagnet FeGa2S4

Spin dynamics in the van der Waals antiferromagnet FeGa$_2$S$_4$ with triangular lattices are investigated using magnetometry, neutron scattering, and muon spin relaxation measurements. The characteristic spin relaxation time is thoroughly clarified over thirteen orders of magnitude. Although the temperature dependence of DC and AC susceptibilities recalls a conventional spin-glass transition, nonlinear susceptibilities showing no divergences at the anomalous temperature, $T^{\ast}=16.87(7)$~K, deny that and instead hint at other mechanisms. Elastic neutron scattering together with previously measured muon results depict a slowly fluctuated ($\sim 10^{-5}$~sec) spin state above $T^{\ast}$. In juxtaposing the underlying simplest structure among frustrated magnets with an intricate hierarchy of time scales, FeGa$_2$S$_4$ can be a playground for studying temporal spin correlations in the two-dimensional limit.

cond-mat.str-el

Chiral-Split Magnon in Altermagnetic MnTe

Altermagnetism is a newly discovered magnetic class named after the alternating spin polarizations in both real and reciprocal spaces. Like the spin-splitting of electronic bands, the magnon bands in altermagnets are predicted to exhibit alternating chiral splitting. In this work, by performing inelastic neutron scattering on $α$-MnTe, we directly verified the chiral splitting in altermagnetic magnon dispersions. The lifted degeneracy of chirality is further explained by a symmetric-exchange origin. In addition, the $g$-wave magnetism was identified in MnTe.

cond-mat.str-el

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

A new inelastic neutron spectrometer HODACA

A new multiplex-type inelastic neutron scattering spectrometer, HOrizontally Defocusing Analyzer Concurrent data Acquisition spectrometer (HODACA), was recently developed and built at the C1-1 cold neutron beam port in JRR-3. The spectrometer is suitable for dynamics measurements in the energy range of $-1$ meV $\lesssim \hbar ω\lesssim$ 7 meV, catering to a broad array of research fields in physics and material science. HODACA combines 24 detectors and 132 pieces of analyzer crystals and has an estimated measurement efficiency that is 70 times greater than the existing conventional triple-axis spectrometer at the C1-1 beam port. The concept, design, specification, and results of commissioning experiments are described.

physics.ins-det

Non-Conventional Critical Behavior and Q-dependent Electron-Phonon Coupling Induced Phonon Softening in the CDW Superconductor LaPt2Si2

This paper reports the first experimental observation of phonons and their softening on single crystalline LaPt$_2$Si$_2$ via inelastic neutron scattering. From the temperature dependence of the phonon frequency in close proximity to the charge-density wave (CDW) $q$-vector, we obtain a CDW transition temperature of T$_{CDW}$ = 230 K and a critical exponent $β$ = 0.28 $\pm$ 0.03. This value is suggestive of a non-conventional critical behavior for the CDW phase transition in LaPt$_2$Si$_2$, compatible with a scenario of CDW discommensuration (DC). The DC would be caused by the existence of two CDWs in this material, propagating separately in the non equivalent (Si1-Pt2-Si1) and (Pt1-Si2-Pt1) layers respectively, with transition temperatures T$_{CDW-1}$ = 230 K and T$_{CDW-2}$ = 110 K. A strong $q$-dependence of the electron-phonon coupling has been identified as the driving mechanism for the CDW transition at T$_{CDW-1}$ = 230 K while a CDW with 3-dimensional character, and Fermi surface quasi-nesting as a driving mechanism, is suggested for the transition at T$_{CDW-2}$ = 110 K. Our results clarify some aspects of the CDW transition in LaPt$_2$Si$_2$, which have been so far misinterpreted by both theoretical predictions and experimental observations, and give direct insight into its actual temperature dependence.

cond-mat.supr-con

Inelastic Neutron Scattering in Weakly Coupled Triangular Spin Tubes CsCrF$_4$

We performed inelastic neutron scattering (INS) experiments to measure spin dynamics on a polycrystalline sample of a spin tube candidate CsCrF$_{4}$. The compound exhibits a successive phase transition from a paramagnetic phase through an intermediate temperature (IT) phase of a 120$^{\circ}$ structure to a low temperature (LT) phase of another 120$^{\circ}$ structure. Elaborate comparison between observed and calculated neutron spectra in LT phase reveals that the spin Hamiltonian is identified as antiferromagnetic spin tubes including perturbative terms of intertube interaction, Dzyaloshinskii-Moriya interaction, and single ion anisotropy. A phase diagram for the ground state is classically calculated. A set of parameters in the spin Hamiltonian obtained from the INS spectra measured in LT phase is quite close to a boundary to the phase of the 120$^{\circ}$ structure of IT phase. The INS spectra measured in IT phase is, surprisingly, the same as those in LT phase in the level of powder averaged spectra, even though the magnetic structures in IT and LT phases are different. Identical dynamical structures compatible with two different static structures are observed. No difference in the observed spectra indicates no change of the spin Hamiltonian with the temperature, suggesting that the origin of the successive phase transition being order-by-disorder mechanism.

cond-mat.other

Spin Excitation in Coupled Honeycomb Lattice Ni$_2$InSbO$_6$

We performed an inelastic neutron scattering experiment on a polycrystalline sample of a helimagnet Ni$_2$InSbO$_6$ to construct the spin Hamiltonian. Well-defined spin-wave excitation with a band energy of 20 meV was observed below $T_{N} = 76$ K. Using the linear spin-wave theory, the spectrum was reasonably reproduced with honeycomb spin layers coupled along the stacking axis (the $c$ axis). The proposed spin model reproduces the soliton lattice induced by a magnetic field applied perpendicular to the $c$ axis.

cond-mat.str-el

Antiferromagnetic Kitaev interaction in $J_\rm{eff}=1/2$ cobalt honeycomb materials Na$_3$Co$_2$SbO$_6$ and Na$_2$Co$_2$TeO$_6$

Finding new materials with antiferromagnetic (AFM) Kitaev interaction is an urgent issue to broaden and enrich the quantum magnetism research significantly. By carrying out inelastic neutron scattering experiments and subsequent analysis, we conclude that Na$_3$Co$_2$SbO$_6$ and Na$_2$Co$_2$TeO$_6$ are new honeycomb cobalt-based AFM Kitaev systems. The spin-orbit excitons at 20-28~meV in both compounds strongly supports the idea that Co$^{2+}$ ions of both compounds have a spin-orbital entangled $J_\rm{eff}=1/2$ state. Furthermore, we found that a generalized Kitaev-Heisenberg Hamiltonian can well describe the spin-wave excitations of both compounds with additional 3rd nearest-neighbor interaction. Our best-fit parameters show large AFM Kitaev terms and off-diagonal symmetric anisotropy terms of a similar magnitude in both compounds. We should stress that our parameters' optimized magnetic structures are consistent with the magnetic structures reported from neutron diffraction studies. Moreover, there is also the magnon-damping effect at the higher energy part of the spin waves, as usually observed in other Kitaev magnets. We demonstrate that Na$_3$Co$_2$SbO$_6$ and Na$_2$Co$_2$TeO$_6$ are the first experimental realization of AFM Kitaev magnets based on the systematic studies of the spin waves and analysis.

cond-mat.str-el

Field-induced quantum spin disordered state in spin-1/2 honeycomb magnet Na2Co2TeO6

Spin-orbit coupled honeycomb magnets with the Kitaev interaction have received a lot of attention due to their potential of hosting exotic quantum states including quantum spin liquids. Thus far, the most studied Kitaev systems are 4d/5d-based honeycomb magnets. Recent theoretical studies predicted that 3d-based honeycomb magnets, including Na2Co2TeO6 (NCTO), could also be a potential Kitaev system. Here, we have used a combination of heat capacity, magnetization, electron spin resonance measurements alongside inelastic neutron scattering (INS) to study NCTO's quantum magnetism, and we have found a field-induced spin disordered state in an applied magnetic field range of 7.5 T < B (vertical to b-axis) < 10.5 T. The INS spectra were also simulated to tentatively extract the exchange interactions. As a 3d-magnet with a field-induced disordered state on an effective spin-1/2 honeycomb lattice, NCTO expands the Kitaev model to 3d compounds, promoting further interests on the spin-orbital effect in quantum magnets.

cond-mat.str-el

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

Nontrivial temperature dependence of magnetic anisotropy in multiferroics Ba$_2$MnGe$_2$O$_7$

We measured the temperature dependences of the static magnetization and the spin excitation in a square-lattice multiferroics Ba$_2$MnGe$_2$O$_7$. An anisotropy gap of the observed low energy mode is scaled by electric polarization rather than a power of sublattice moment. Spin nematic interaction in effective spin Hamiltonian, which is equivalent to interaction of electric polarization, is responsible for the easy-axis anisotropy. The nontrivial behavior of the anisotropy gap can be rationalized as change of the hybridized $d$-$p$ orbital with temperature, leading to the temperature dependence of the spin nematic interaction.

cond-mat.str-el

Spin-gap formation due to spin-Peierls instability in $π$-orbital-ordered NaO$_2$

We have investigated the low-temperature magnetism of sodium superoxide (NaO$_{2}$), in which spin, orbital, and lattice degrees of freedom are closely entangled. The magnetic susceptibility shows anomalies at $T_{1}=220$ K and $T_{2}=190$ K, which correspond well to the structural phase transition temperatures, and a sudden decrease below $T_{3}=34$ K. At 4.2 K, the magnetization shows a clear stepwise anomaly around 30 T with a large hysteresis. In addition, the muon spin relaxation experiments indicate no magnetic phase transition down to $T=0.3$ K. The inelastic neutron scattering spectrum exhibits magnetic excitation with a finite energy gap. These results confirm that the ground state of NaO$_{2}$ is a spin-singlet state. To understand this ground state in NaO$_{2}$, we performed Raman scattering experiments. All the Raman-active libration modes expected for the marcasite phase below $T_{2}$ are observed. Furthermore, we find that several new peaks appear below $T_{3}$. This directly evidences the low crystal symmetry, namely, the presence of the phase transition at $T_{3}$. We conclude the singlet-ground state of NaO$_{2}$ due to the spin-Peierls instability.

cond-mat.str-el

Spin-waves in 2D honeycomb lattice $XXZ$-type van der Waals antiferromagnet CoPS$_3$

The magnetic excitations in CoPS$_3$, a two-dimensional van der Waals (vdW) antiferromagnet with spin $S=3/2$ on a honeycomb lattice, has been measured using powder inelastic neutron scattering. Clear dispersive spin waves are observed with a large spin gap of ~13 meV. The magnon spectra were fitted using an $XXZ$-type $J_1-J_2-J_3$ Heisenberg Hamiltonian with a single-ion anisotropy assuming no magnetic exchange between the honeycomb layers. The best-fit parameters show ferromagnetic exchange $J_1=-2.08$ meV and $J_2=-0.26$ meV for the nearest and second-nearest neighbors and a sizeable antiferromagnetic exchange $J_3=4.21$ meV for the third-nearest neighbor with the strong easy-axis anisotropy $K=-2.06$ meV. The suitable fitting could only be achieved by the anisotropic $XXZ$-type Hamiltonian, in which the exchange interaction for the out-of-plane component is smaller than that for the in-plane one by a ratio $α=J_z/J_x=0.6$. Moreover, the absence of spin-orbit exciton around 30 meV indicates that Co$^{2+}$ ions in CoPS$_3$ have a $S=3/2$ state rather than a spin-orbital entangled $J_\rm{eff}=1/2$ ground state. Our result directly shows that CoPS$_3$ is an experimental realization of the $XXZ$ model with a honeycomb lattice in 2D vdW magnets.

cond-mat.mtrl-sci