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Gakuto Kusuno

Publications and source records attributed to Gakuto Kusuno.

7 recordsLinked to original sources

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

Quantifying chirality of phonons

Recent years have witnessed growing interest in chiral phonons, lattice vibrations carrying angular momentum and exhibiting handedness, as revealed by helicity-dependent optical phenomena. Despite this progress, a quantitative characterization of phonon chirality as a dynamical property has remained elusive. In this work, we propose a theoretical framework to quantify the dynamical chirality of lattice vibrations. We introduce two quantitative measures: momentum-resolved dynamical chirality, which provides a mode- and wave-vector-resolved picture of phonon chirality, and the bulk dynamical chirality, which characterizes the collective behavior of thermally populated chiral phonons. Using first-principles calculations for both chiral and achiral materials, we demonstrate how these quantities capture the handedness and population imbalance of phonon modes and serve as a means to distinguish the enantiomers of chiral crystals.

cond-mat.mtrl-sci

Electric toroidal octupolar symmetry in pyrite FeS$_2$ probed by Raman optical activity

We report Raman optical activity in pyrite FeS$_2$, which hosts an electric toroidal octupolar symmetry. A clear and reproducible sign reversal of the circular intensity difference is observed between neighboring $\{111\}$ faces under cross-circular polarization. The signal appears only for the doubly degenerate $E_g$ phonon mode and is absent for other modes, consistent with symmetry analysis. First-principles calculations reproduce these features, establishing Raman optical activity as a probe of higher-rank axial multipolar symmetry.

cond-mat.mtrl-sci

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

Polarization-dependent photocurrent in a quadrilateral-shaped bulk crystalline tellurium chip with near-infrared light excitation

We report the detection of zero-bias photocurrents induced by interband excitation using oblique near-infrared light (λ=0.780 μm) along the directions parallel and perpendicular to the helical axis in a millimeter-sized Te crystal. The photocurrent parallel to the helical axis exhibits a circular-polarization-dependent component, namely circular photogalvanic effect. We create a framework for estimating the gyrotropic photoconductivity tensor \b{eta}, the ratio between the circular-polarization-dependent photocurrent density and intensity of light, through which extrinsic \b{eta} values ranging from a few to a few tens of nA/W are obtained. Searching the \b{eta} values through existing literatures reveals that these values vary significantly with sample conditions, excitation wavelengths, and forms of crystallite samples. A particular interesting point found in our study is that the \b{eta} values for the interband excitation may be greater than those for intraband excitation as far as bulk Te is concerned.

cond-mat.mtrl-sci

Symmetry analysis of cross-circular and parallel-circular Raman optical activity

The Raman scattering regarding the circularly-polarized incident and scattered lights is closely related to the circular activity of a given system. We investigate the symmetry of its activity, called the cross-circular and parallel-circular Raman optical activity. The analysis is systematically performed with the magnetic point groups and indicates that the response allows for a useful diagnosis of the symmetry of materials like chirality and (magneto-)axiality. It is also shown that the Stokes and anti-Stokes processes are related to each other by the conserved antiunitary symmetry for the time-reversal operation and that combined with the mirror reflection.

cond-mat.mtrl-sci

Raman Optical Activity Induced by Ferroaxial Order in NiTiO$_3$

Raman optical activity (ROA), the dependence of Raman intensity on the circular polarization of incident and scattered light, has traditionally been observed in chiral molecules and magnetic materials, where inversion or time-reversal symmetry is broken. Here we demonstrate that ROA can also arise in a centrosymmetric and non-magnetic ferroaxial crystal. Using circularly polarized Raman spectroscopy on single-crystalline NiTiO$_3$, we observed a pronounced ROA signal in the cross-circular polarization configurations, which correlates with the ferroaxial domain structure. Our symmetry analysis, first-principles calculations of phonons, and tight-binding model calculations reveal that the natural ROA originates from the ferroaxial order and persists even within the electric dipole approximation. These results establish ROA as a powerful probe of ferroaxial order in centrosymmetric systems.

cond-mat.mtrl-sci