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Yusuke Kousaka

Publications and source records attributed to Yusuke Kousaka.

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Emergence of Chiral Helimagnetic Order in Chromium-intercalated Tantalum Disulfide CrTa$_3$S$_6$ Powders with Controlled Intercalation

We report a highly sensitive change in magnetic properties of a chiral Cr-intercalated transition-metal dichalcogenide Cr$_{x}$Ta$_{3}$S$_{6}$. Magnetization curves and small-angle neutron scattering data revealed that the powder samples exhibit chiral helimagnetism with a Cr intercalation quantity $x$ below 0.996, while they show ferromagnetism above 1.000. The emergence and temperature-dependent evolution of the helimagnetic period are argued in terms of sample dimensions of powders and microfabricated crystals.

cond-mat.mtrl-sci

Circular Raman responses from angular-momentum inequivalence in CoSi

Circularly polarized Raman scattering in solids exhibits distinct phenomena such as Raman optical activity (ROA) and chiral-phonon-induced frequency splitting, whose relationship has remained unclear. Here we show that these seemingly different responses can be understood within a common framework based on the inequivalence of phonon states carrying opposite crystal angular momenta. Using helicity-resolved Raman spectroscopy of the chiral crystal CoSi, we find that ROA and frequency splitting arise from different symmetry channels, namely axial multipolar symmetry and structural chirality, respectively. First-principles calculations reproduce both effects and clarify their symmetry origins. These results establish angular-momentum inequivalence as a unifying principle of circular Raman responses and link helicity-resolved Raman spectroscopy to the angular-momentum structure of chiral phonons in topological materials.

physics.optics

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/$\mu_{\rm B}$. 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 $\beta\simeq 0.23$, 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 $\nu_Q=32.72(5)$ 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

Chiral phonons in sixfold chiral CrSi$_2$: Raman spectroscopy and first-principles calculations

Chiral phonons have been identified in several chiral crystals, primarily in those with trigonal symmetry and threefold screw axes. In this study, chiral phonons in CrSi$_2$, a chiral crystal with a sixfold helical structure, were investigated. Circularly polarized Raman spectroscopy revealed a subtle splitting of doubly degenerate $E_2$ phonon modes between cross-circular polarization configurations. These observations, supported by first-principles phonon calculations, indicate the presence of chiral phonons in CrSi$_2$, expanding the scope of materials that exhibit chiral vibrational modes beyond the conventional trigonal class.

cond-mat.mtrl-sci

Spin phase detection by spin current in a chiral helimagnet

Helimagnets, characterized by a helical arrangement of magnetic moments, possess unique internal degrees of freedom, including the spin phase, defined by the phase of the helical magnetic structure. Electrical detection of the spin phase is essential for both practical applications and fundamental research in helimagnets. Here, we demonstrate the electrical detection of the spin phase in a van der Waals nanoscale chiral helimagnet CrNb$_3$S$_6$ using nonlocal spin valve measurements. Due to the short spin diffusion length in CrNb$_3$S$_6$ ($\sim5$~nm), the surface magnetic moment direction, which corresponds to the spin phase, can be detected via spin currents. The experimentally observed magnetic field dependence of the nonlocal spin valve signal is consistent with that of the surface magnetic moment in the helical magnetic structure, as supported by micromagnetic simulations. Our results establish spin currents as a powerful tool for detecting the spin phase in helimagnets, opening avenues for utilizing the spin phase as a novel internal degree of freedom in nanoscale spintronic devices.

cond-mat.mes-hall

Superconductivity in Ternary Germanite TaAl$_{x}$Ge$_{2-x}$ with a C40 chiral structure

We report a new family of chiral intermetallic superconductors TaAl$_{x}$Ge$_{2-x}$. The mother compound TaGe$_2$ has a C40-type chiral hexagonal crystal structure with a pair of enantiomorphic space groups of $P6{_2}22$ and $P6{_4}22$. By substituting Ge with Al, TaAl$_{x}$Ge$_{2-x}$ polycrystals with the C40 structure were synthesized with Al substitution $x$ from 0 to 0.8. Magnetic susceptibility, magnetization curves and electrical resistivity revealed that TaAl$_{x}$Ge$_{2-x}$ with $x$ of 0.2 to 0.4 was a type-II superconductor with a superconducting transition temperature $T_{\rm c}$ of 2.0 to 2.2 K. The superconductivity disappeared or was largely suppressed at $x$ less than 0.2 and more than 0.4, although all the measurements were performed at temperatures above 1.8 K. An emergence of superconductivity is discussed in terms of the lattice constants changes with the Al substitution.

cond-mat.supr-con

Spin polarization gate device based on the chirality-induced spin selectivity and robust nonlocal spin polarization

Nonlocal spin polarization phenomena are thoroughly investigated in the devices made of chiral metallic single crystals of CrNb$_3$S$_6$ and NbSi$_2$ as well as of polycrystalline NbSi$_2$. We demonstrate that simultaneous injection of charge currents in the opposite ends of the device with the nonlocal setup induces the switching behavior of spin polarization in a controllable manner. Such a nonlocal spin polarization appears regardless of the difference in the materials and device dimensions, implying that the current injection in the nonlocal configuration splits spin-dependent chemical potentials throughout the chiral crystal even though the current is injected into only a part of the crystal. We show that the proposed model of the spin dependent chemical potentials explains the experimental data successfully. The nonlocal double-injection device may offer significant potential to control the spin polarization to large areas because of the nature of long-range nonlocal spin polarization in chiral materials.

cond-mat.mtrl-sci

Chiral phonons: circularly polarized Raman spectroscopy and $\textit{ab initio}$ calculations in a chiral crystal tellurium

Recently, phonons with chirality (chiral phonons) have attracted significant attention. Chiral phonons exhibit angular and pseudo-angular momenta. In circularly polarized Raman spectroscopy, the peak split of the $Γ_3$ mode is detectable along the principal axis of the chiral crystal in the backscattering configuration. In addition, peak splitting occurs when the pseudo-angular momenta of the incident and scattered circularly polarized light are reversed. Until now, chiral phonons in binary crystals have been observed, whereas those in unary crystals have not been observed. Here, we observe chiral phonons in a chiral unary crystal Te. The pseudo-angular momentum of the phonon is obtained in Te by an $\textit{ab initio}$ calculation. From this calculation, we verified the conservation law of pseudo-angular momentum in Raman scattering. From this conservation law, we determined the handedness of the chiral crystals. We also evaluated the true chirality of the phonons using a measure with symmetry similar to that of an electric toroidal monopole.

cond-mat.mtrl-sci

Chirality-selected crystal growth and spin polarization over centimeters of transition metal disilicide crystals

We performed a chirality-controlled crystal growth of transition metal disilicide NbSi$_{2}$ and TaSi$_{2}$ by using a laser-diode-heated floating zone (LDFZ) method. The crystal chirality was evaluated in the crystals of centimeters in length by performing single crystal X-ray diffraction as well as probing a spin polarization originating from chirality-induced spin selectivity (CISS) effect. The crystals of right-handed NbSi$_{2}$ and of left-handed TaSi$_{2}$ were obtained in the conventional LDFZ crystal growth, while the left-handed NbSi$_{2}$ and right-handed TaSi$_{2}$ crystals were grown by the LDFZ method with the composition-gradient feed rods. The spin polarization via the CISS was observed over centimeters in the NbSi$_{2}$ single crystals and the sign of the CISS signals was dependent on the chirality of crystals. The correlation between the crystal chirality and CISS signals indicates that the CISS measurements work as a non-destructive method for chirality determination even in centimeter-long specimens.

cond-mat.mtrl-sci

Truly chiral phonons in α-HgS

Chirality is a manifestation of the asymmetry inherent in nature. It has been defined as the symmetry breaking of the parity of static objects, and the definition was extended to dynamic motion such that true and false chiralities were distinguished. Recently, rotating, yet not propagating, atomic motions were predicted and observed in two-dimensional materials, and they were referred to as "chiral phonons" . A natural development would be the discovery of truly chiral phonons that propagate while rotating in three-dimensional materials. Here, we used circularly polarised Raman scattering and first-principles calculations to identify truly chiral phonons in chiral bulk crystals. This approach enabled us to determine the chirality of a crystal in a non-contact and non-destructive manner. In addition, we demonstrated that the law of the conservation of pseudo-angular momentum holds between circularly polarised photons and chiral phonons. These findings are expected to help develop ways for transferring the pseudo-angular momentum from photons to electron spins via the propagating chiral phonons in opto-phononic-spintronic devices.

cond-mat.mtrl-sci

Chirality-Controlled Enantiopure Crystal Growth of a Transition Metal Monosilicide by a Floating Zone Method

We performed a crystal growth to obtain chirality-controlled enantiopure crystals using a laser-diode-heated floating zone (LDFZ) method with a composition-gradient feed rod. It has been argued that the crystal handedness of $T$Si ($T$ : transition metal) is fixed depending on $T$ in the case of the ones grown by the conventional methods. We found that right-handed single crystals of CoSi and MnSi were grown from the composition gradient feed rods that consist of FeSi--CoSi and FeSi--MnSi, respectively. The obtained CoSi and MnSi crystals inherit the chirality from the seed part of FeSi, which grows in a right-handed structure, and thus have the chirality opposite to that for the crystals in the literature. The LDFZ method with the feed rods with various combinations of $T$Si compounds enables a flexible control of the chirality of $T$Si and will be useful for clarifying the interplay between the crystalline chirality and chirality-induced physical responses.

cond-mat.mtrl-sci

Momentum-dependent magnon lifetime in the metallic non-collinear triangular antiferromagnet CrB2

Non-collinear magnetic order arises for various reasons in several magnetic systems and exhibits interesting spin dynamics. Despite its ubiquitous presence, little is known of how magnons, otherwise stable quasiparticles, decay in these systems, particularly in metallic magnets. Using inelastic neutron scattering, we examine the magnetic excitation spectra in a metallic non-collinear antiferromagnet CrB$_{2}$, in which Cr atoms form a triangular lattice and display incommensurate magnetic order. Our data show intrinsic magnon damping and continuum-like excitations that cannot be explained by linear spin wave theory. The intrinsic magnon linewidth $Γ(q,E_{q})$ shows very unusual momentum dependence, which our analysis shows to originate from the combination of two-magnon decay and the Stoner continuum. By comparing the theoretical predictions with the experiments, we identify where in the momentum and energy space one of the two factors becomes more dominant. Our work constitutes a rare comprehensive study of the spin dynamics in metallic non-collinear antiferromagnets. It reveals, for the first time, definite experimental evidence of the higher-order effects in metallic antiferromagnets.

cond-mat.str-el

Order and Disorder in the Magnetisation of the Chiral Crystal CrNb$_3$S$_6$

Competing magnetic anisotropies in chiral crystals with Dzyaloshinskii Moriya exchange interactions can give rise to non-trivial chiral topological magnetisation configurations with new and interesting properties. One such configuration is the magnetic soliton, where the moment continuously rotates about an axis. This magnetic system can be considered to be one dimensional and, because of this, it supports a macroscale coherent magnetisation, giving rise to a tunable chiral soliton lattice (CSL) that is of potential use in a number of applications in nanomagnetism and spintronics. In this work we characterise the transitions between the forced-ferromagnetic (F-FM) phase and the CSL one in CrNb$_3$S$_6$ using differential phase contrast imaging in a scanning transmission electron microscope, conventional Fresnel imaging, ferromagnetic resonance spectroscopy, and mean-field modelling. We find that the formation and movement of dislocations mediate the formation of CSL and F-FM regions and that these strongly influence the highly hysteretic static and dynamic properties of the system. Sample size and morphology can be used to tailor the properties of the system and, with the application of magnetic field, to locate and stabalise normally unstable dislocations and modify their dimensions and magnetic configurations in ways beyond that predicted to occur in uniform films.

cond-mat.mtrl-sci

Nucleation, instability, and discontinuous phase transitions in monoaxial helimagnets with oblique fields

The phase diagram of the monoaxial chiral helimagnet as a function of temperature (T ) and magnetic field with components perpendicular (H x ) and parallel (H z ) to the chiral axis is theoretically studied via the variational mean field approach in the continuum limit. A phase transition surface in the three dimensional thermodynamic space separates a chiral spatially modulated phase from a homogeneous forced ferromagnetic phase. The phase boundary is divided into three parts: two surfaces of second order transitions of instability and nucleation type, in De Gennes terminology, are separated by a surface of first order transitions. Two lines of tricritical points separate the first order surface from the second order surfaces. The divergence of the period of the modulated state on the nucleation transition surface has the logarithmic behavior typical of a chiral soliton lattice. The specific heat diverges on the nucleation surface as a power law with logarithmic corrections, while it shows a finite discontinuity on the other two surfaces. The soliton density curves are described by a universal function of H x if the values of T and H z determine a transition point lying on the nucleation surface; otherwise, they are not universal.

cond-mat.str-el

Chiral Soliton Lattice Formation in Monoaxial Helimagnet Yb(Ni$_{1-x}$Cu$_x$)$_3$Al$_9$

Helical magnetic structures and its responses to external magnetic fields in Yb(Ni$_x$Cu$_{1-x}$)$_3$Al$_9$, with a chiral crystal structure of the space group $R32$, have been investigated by resonant X-ray diffraction. It is shown that the crystal chirality is reflected to the helicity of the magnetic structure by a one to one relationship, indicating that there exists an antisymmetric exchange interaction mediated via the conduction electrons. When a magnetic field is applied perpendicular to the helical axis ($c$ axis), the second harmonic peak of $(0, 0, 2q)$ develops with increasing the field. The third harmonic peak of $(0, 0, 3q)$ has also been observed for the $x$=0.06 sample. This result provides a strong evidence for the formation of a chiral magnetic soliton lattice state, a periodic array of the chiral twist of spins, which has been suggested by the characteristic magnetization curve. The helical ordering of magnetic octupole moments, accompanying with the magnetic dipole order, has also been detected.

cond-mat.str-el

Understanding the H-T phase diagram of the mono-axial helimagnet

Some unexpected features of the phase diagram of the monoaxial helimagnet in presence of an applied magnetic field perpendicular to the chiral axis are theoretically predicted. A rather general hamiltonian with long range Heisenberg exchange and Dzyaloshinskii--Moriya interactions is considered. The continuum limit simplifies the free energy, which contains only a few parameters which in principle are determined by the many parameters of the hamiltonian, although in practice they may be tuned to fit the experiments. The phase diagram contains a Chiral Soliton Lattice phase and a forced ferromagnetic phase separated by a line of phase transitions, which are of second order at low T and of first order in the vicinity of the zero-field ordering temperature, and are separated by a tricritical point. A highly non linear Chiral Soliton Lattice, in which many harmonics contribute appreciably to the spatial modulation of the local magnetic moment, develops only below the tricritical temperature, and in this case the scaling shows a logarithmic behaviour similar to that at T=0, which is a universal feature of the Chiral Soliton Lattice. Below the tricritical temperature, the normalized soliton density curves are found to be independent of T, in agreement with the experimental results of magnetorresistance curves, while above the tricritical temperature they show a noticeable temperature dependence. The implications in the interpretation of experimental results of CrNb3S6 are discussed.

cond-mat.str-el

Incommensurate--commensurate transitions in the mono-axial chiral helimagnet driven by the magnetic field

The zero temperature phase diagram of the mono-axial chiral helimagnet in the magnetic field plane formed by the components parallel and perpendicular to the helical axis is thoroughly analyzed. The nature of the transition to the commensurate state depends on the angle between the field and the helical axis. For field directions close to the directions parallel or perpendicular to the helical axis the transition is continuous, while for intermediate angles the transition is discontinuous and the incommensurate and commensurate states coexist on the transition line. The continuous and discontinuous transition lines are separated by two tricritical points with specific singular behaviour. The location of the continuous and discontinuous lines and of the tricritical points depend strongly on the easy-plane anisotropy, the effect of which is analyzed. For large anisotropy the conical approximation locates the transition line very accurately, although it does not predict the continuous transitions nor the tricitical behaviour. It is shown that for large anisotropy, as in CrNb3S6, the form of the transition line is universal, that is, independent of the sample, and obeys a simple equation. The position of the tricritical points, which is not universal, is theoretically estimated for a sample of CrNb3S6

cond-mat.str-el

Observation of elastic anomalies driven by coexisting dynamical spin Jahn-Teller effect and dynamical molecular spin state in paramagnetic phase of the frustrated MgCr$_2$O$_4$$

Ultrasound velocity measurements of magnesium chromite spinel MgCr$_2$O$_4$ reveal elastic anomalies in the paramagnetic phase that are characterized as due to geometrical frustration. The temperature dependence of the tetragonal shear modulus $(C_{11}-C_{12})/2$ exhibits huge Curie-type softening, which should be the precursor to spin Jahn-Teller distortion in the antiferromagnetic phase. The trigonal shear modulus $C_{44}$ exhibits nonmonotonic temperature dependence with a characteristic minimum at $\sim$50 K, indicating a coupling of the lattice to dynamical molecular spin state. These results strongly suggest the coexistence of dynamical spin Jahn-Teller effect and dynamical molecular spin state in the paramagnetic phase, which is compatible with the coexistence of magnetostructural order and dynamical molecular spin state in the antiferromagnetic phase.

cond-mat.str-el