arXiv subjects

Rikuto Oiwa

Publications and source records attributed to Rikuto Oiwa.

At least 19 recordsLinked to original sources

arXiv2026

Observation of g-wave altermagnetic multipole

Over the past few years, altermagnets have emerged as a new class of collinear magnets with broken time-reversal symmetry, offering novel opportunities for spintronics beyond conventional magnets. Rather than from net magnetization, as in ferromagnets, the unconventional time-reversal symmetry breaking of altermagnets originates from antiferroic magnetic dipoles locked to higher-order multipoles. Here we report the direct visualization of a $g$-wave altermagnetic multipole in the canonical altermagnet CrSb. Combining high-energy synchrotron X-ray diffraction with valence electron density (VED) analysis, we uncover a pronounced directional anisotropy of the VED distribution alternating between Cr sublattices. This evidences the antiferroic order of electric hexadecapoles predicted in $g$-wave altermagnets. Its coexistence with antiferroic magnetic dipoles induces ferroic magnetic multipoles, as probed by polarized neutron diffraction. We further identify a microscopic model of altermagnetism that directly relates the $g$-wave multipole and the $g$-wave spin splitting. Through direct observation and quantification of multipoles, this study provides a real-space fingerprint of altermagnetism and establishes a general probe of hidden multipole order in quantum materials.

cond-mat.str-el↗

arXiv2026

Sixteenfold Classification of Many-Body Multipoles from Rotation-Compatible Canonical Symmetries

The conventional multipole framework provides a standard symmetry-based language for one-body electronic degrees of freedom, but fails to distinguish physically distinct sectors in many-body operator space. We show that canonical symmetries compatible with rotations provide this structure through two additional 2 labels associated with the particle-number gauge transformation Gπ/2 and the particle-hole transformation CA. These labels separate operators with different body numbers and particle-number changes, leading to a sixteenfold classification that organizes selection rules for nonzero expectation values, induced multipoles, and symmetry-allowed couplings in many-body multipole space.

cond-mat.str-el↗

arXiv2026

Piezoaxial coupling for strain-selected ferroaxial domain control

We formulate a symmetry-based hierarchy of strain-derived conjugate fields for ferroaxial order, and demonstrate strain-selected ferroaxial domain control using first-principles calculations. Since ferroaxial order is even under both spatial inversion and time reversal, ordinary electric and magnetic fields cannot serve as universal linear conjugate fields. Homogeneous strain, however, can generate symmetry-allowed piezoaxial fields whose leading order is determined by the parent point group and by the chosen ferroaxial-axis component. For basal-plane strain, the leading field is linear in orthorhombic systems, quadratic in tetragonal systems, and cubic in trigonal and hexagonal systems. Cubic parent groups further split into two classes: cubic-I groups, $23$ and $m\bar{3}$, allow linear full-strain fields for selected axes, whereas cubic-II groups, $432$, $\bar{4}3m$, and $m\bar{3}m$, forbid linear fields and require quadratic or cubic strain combinations depending on the selected axis. In trigonal systems, the basal-plane deviatoric strain with signed amplitude $\varepsilon_{\rm u}$ and principal-axis angle $θ$ gives the single-axis field $h\propto\varepsilon_{\rm u}^3\sin6θ$. First-principles calculations for the trigonal ferroaxial compound Na$_2$BaMg(PO$_4$)$_2$ verify both the predicted angular dependence and cubic strain scaling of the ferroaxial domain splitting, and fixed-strain atomic relaxations show strain-selected evolution from the para-axial structure. These results establish static homogeneous strain as a symmetry-allowed conjugate field for ferroaxial order and suggest a route to ferroaxial domain control through strain-field cooling.

cond-mat.mtrl-sci↗

arXiv2026

Theory of Many-Body Multipole Operators in Single-Centered Electron Systems: Two-Body Toroidal Monopoles in Spinless Orbitals

One-body multipole operators are defined as irreducible representations of rotational symmetry together with spatial-inversion and time-reversal symmetries, providing a systematic framework for classifying electronic internal degrees of freedom and for describing a wide variety of composite order parameters. While this formalism has been successfully established for the one-body operator space, a systematic classification of the many-body operator space, especially in interacting systems, remains an open challenge. In this paper, we extend the multipole formalism in the one-body operator space to the many-body operator space. By formulating fermionic creation and annihilation operators as spherical tensors and employing Clebsch-Gordan coupling combined with the exterior (Grassmann) algebra, we construct an irreducible decomposition of many-body operators that fully incorporates fermionic antisymmetrization. As a concrete application, we classify monopoles appearing in spinless many-body operators. In particular, we show that the electric toroidal monopole, a pseudoscalar breaking spatial-inversion symmetry, and the magnetic toroidal monopole, a time reversal-odd scalar, become active in spinless interacting many-body systems, although they are absent in the spinless one-body hybrid orbital space.

cond-mat.str-el↗

arXiv2026

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↗

arXiv2026

Effective phonon models based on symmetry-adapted multipole basis -- Hidden chiral phonon angular momentum splitting in ferroaxial systems

We propose a symmetry-based framework for constructing effective harmonic phonon models using a symmetry-adapted multipole basis. By decomposing the force-constant matrix into bond-centered electric multipoles, we identify the minimal microscopic ingredients responsible for phonon angular-momentum splitting. Applying this framework to a minimal zigzag-chain model, we show that ferroaxial order gives rise to a hidden sublattice-resolved chiral phonons, while an additional polar contribution leads to finite global chirality. Our results provide a unified symmetry-based description of hidden and emergent phonon phenomena and suggest a route to control phonon properties via electronic orderings and external fields.

cond-mat.mtrl-sci↗

arXiv2026

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↗

arXiv2026

Dual-circular Raman optical activity of axial multipolar order

Multipolar order, such as octupolar order, is a key concept in condensed matter physics, particularly in light of elusive hidden orders. However, its experimental identification remains challenging due to the absence of direct coupling to conventional external stimuli. In this study, we propose that dual-circular Raman scattering serves as a probe of multipolar anisotropies. By combining symmetry analysis with microscopic calculations, we identify that both time-reversal-even ($θ$-even) and time-reversal-odd ($θ$-odd) axial multipolar phases exhibit the sizable Raman optical activity as a direct consequence of multipolar symmetry breaking. The quantitative significance of the proposed response is demonstrated by the first-principles study of pyrite, a prototypical axial octupolar material. Furthermore, we reveal that a multipolar phonon, a three-dimensional and alternating displacement resembling the chiral phonon, plays a vital role in the proposed optical phenomena. Our findings open a pathway for identifying multipolar orders in various materials through dual-circular Raman spectroscopy as a sensitive and versatile probe.

physics.optics↗

arXiv2026

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↗

arXiv2025

Spinless electric toroidal multipoles in ferroaxial ${\rm K_2Zr(PO_4)_2}$ revealed by symmetry-adapted closest Wannier analysis

From a symmetry perspective, ferroaxial order belongs to the same symmetry as time-reversal-even pseudovectors. Experimentally, ${\rm K_2Zr(PO_4)_2}$ is known to undergo a displacive-type phase transition from a non-ferroaxial to a ferroaxial phase. To identify the key microscopic ingredients driving this transition, we carry out a quantitative analysis combining density-functional theory calculations and symmetry-adapted closest Wannier analysis. As a result, we show that electric toroidal dipole, electric toroidal octupole, and electric hexadecapole, which belong to the same irreducible representation, make dominant contributions to the ferroaxial transition. In particular, we find that spinless electric toroidal octupoles, which originate from spin-independent off-diagonal real hopping between the $p$ orbitals on P and O atoms and between the $d$ orbitals on Zr atoms and $p$ orbitals on O atoms, provide the most significant contributions. Moreover, we explicitly analyze the orbital characters involved in the relevant hybridizations associated with these multipoles. We further show that the relativistic spin--orbit coupling has a negligible influence on the ferroaxial transition. These results demonstrate that spin-independent orbital hybridization between different orbitals on different atoms plays a crucial role in inducing the ferroaxial transition.

cond-mat.mtrl-sci↗

arXiv2025

Chirality/Axiality-Induced Axiality/Chirality via Surface Polarization

In condensed matter physics, a broad spectrum of physical characteristics, such as chirality, axiality, and polarity, arises as a direct consequence of the underlying symmetry of the system. We here theoretically investigate the effective coupling between chirality and axiality at their domain boundaries, mediated by polarity. Based on symmetry considerations and model analyses, we propose the concept of chirality-induced axiality via surface polarization, which refers to a phenomenon where the handedness of chirality selects an axial moment with a particular orientation by lowering its energy at the surface. We further establish the inverse process, termed axiality-induced chirality via surface polarization, whereby axiality in turn dictates the preferred chirality. These reciprocal couplings open a new pathway for stabilizing single-domain states of chirality and axiality. They further imply interfacial functionalities, including the selective adsorption of chiral and axial molecules.

cond-mat.str-el↗

arXiv2025

Detection of ferroic octupole ordering in $d$-wave altermagnetic rutile-type compounds

We propose that X-ray absorption and emission magnetic circular dichroism (XAS-MCD and XES-MCD) are promising measurements to directly detect ferroic higher-rank multipoles as candidate order parameters in altermagnets. Using the sum rules for XES-MCD and connecting them to multipole language, we demonstrate that the expectation value of the magnetic octupole moment is finite in the $d$-wave altermagnetic candidate rutile-type compounds TF$_2$ (T=transition metal). We also perform spectral calculations of XAS-MCD and XES-MCD based on an effective model with a full multiplet approach. While the intensity of the XAS-MCD spectra vanishes, the XES-MCD spectra exhibit finite intensity, whose spectrum becomes opposite by inverting the Nèel vector. These results clearly indicate ferroic magnetic octupole order in these compounds.

cond-mat.str-el↗

arXiv2025

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↗

arXiv2025

Predominant Electronic Order Parameter for Structural Chirality -- Role of Spinless Electronic Toroidal Multipoles

We discuss predominant order parameters for structural chirality, and demonstrate that time-reversal-even axial-quadrupole plays a key role in stabilizing a chiral structure. Using the symmetry-adapted closest Wannier model of the trigonal Te and Se, we quantify the evolution of the spin-independent (spinless) and spin-dependent (spinful) electric toroidal (ET) (axial) multipole moments across the transition from an achiral to a chiral structure. Our results clearly identify that a spin-independent off-diagonal real hopping between $p$ orbitals, which corresponds to the bond-cluster spinless ET quadrupole of $(3z^{2}-r^{2})$ type $G_{u}$, is the predominant order parameter in stabilizing helical structures. We further elucidate that the above itinerant spinless ET quadrupole induces a monopole-like orbital angular momentum texture in the momentum space, which can be observed via circular-dichroism in soft x-ray photoemission spectroscopy measurement. Our findings highlight a critical role of the orbital angular momentum in chiral materials rather than less dominant spin angular momentum arising from the relativistic spin-orbit coupling.

cond-mat.mtrl-sci↗

arXiv2025

Symmetry-adapted closest Wannier modeling based on complete multipole basis set

We have developed a method to construct a symmetry-adapted Wannier tight-binding model based on the closest Wannier formalism and the symmetry-adapted multipole theory. Since the symmetry properties of the closest Wannier functions are common to those of the original atomic orbitals, symmetry-adapted multipole basis (SAMB) can be defined as the complete orthonormal matrix basis set in the Hilbert space of the closest Wannier functions. Utilizing the completeness and orthonormality of SAMBs, the closest Wannier Hamiltonian can be expressed as a linear combination of SAMBs belonging to the identity irreducible representation, thereby fully restoring the symmetry of the system. Moreover, the linear coefficients of each SAMB (model parameters) related to crystalline electric fields, spin-orbit coupling, and electron hoppings are determined through simple matrix projection without any iterative procedure. Thus, this method allows us to unveil mutual interplay among hidden electronic multipole degrees of freedom in the Hamiltonian and numerically evaluate them. We demonstrate the effectiveness of our method by modeling monolayer graphene under a perpendicular electric field, highlighting its utility in symmetrizing the closest Wannier model, quantifying symmetry breaking, and predicting unusual responses. The method is implemented in the open-source Python library SymClosestWannier, with the codes available on GitHub (https://github.com/CMT-MU/SymClosestWannier).

cond-mat.mtrl-sci↗

arXiv2024

Quantification of chirality based on electric toroidal monopole

Chirality ubiquitously appears in nature, however, its quantification remains obscure owing to the lack of microscopic description at the quantum-mechanical level. We propose a way of evaluating chirality in terms of electric toroidal monopole, a practical entity of time-reversal even pseudoscalar (parity-odd) object reflecting relevant electronic wave functions. For this purpose, we analyze a twisted methane at the quantum-mechanical level, showing that the electric toroidal monopoles become a quantitative indicator for chirality. In the twisted methane, we clarify that the handedness of chirality corresponds to the sign of the expectation value of the electric toroidal monopole, and that the most important ingredient is the modulation of the spin-dependent imaginary hopping between the hydrogen atoms, while the relativistic spin-orbit coupling within the carbon atom is irrelevant for chirality.

cond-mat.mtrl-sci↗

arXiv2023

Unconventional Hall effect and magnetoresistance induced by metallic ferroaxial ordering

Transport property under metallic ferroaxial ordering in an external magnetic field is theoretically investigated. After presenting the relation between the magnetoconductivity tensor and ferroaxial moment from the symmetry viewpoint, we analyze the behavior of the unconventional Hall effect and magnetoconductivity for a general five $d$-orbital tight-binding model under the point group $C_{\rm 4h}$, where the ferroaxial moment is activated. We show that the crystalline electric field that arises from the symmetry reduction from $D_{\rm 4h}$ to $C_{\rm 4h}$ is essential for the ferroaxial-related magnetotransport, while the relativistic spin-orbit coupling is not required. We also compare the unconventional Hall effect driven by the ferroaxial moment with the conventional Hall effect, the latter of which does not require the ferroaxial moment. The present results provide characteristic transport properties in the ferroaxial systems, which can be observed in various candidate materials like Ca$_5$Ir$_3$O$_{12}$.

cond-mat.str-el↗

arXiv2023

Symmetry-adapted modeling for molecules and crystals

We have developed a symmetry-adapted modeling procedure for molecules and crystals. By using the completeness of multipoles to express spatial and time-reversal parity-specific anisotropic distributions, we can generate systematically the complete symmetry-adapted multipole basis set to describe any of electronic degrees of freedom in isolated cluster systems and periodic crystals. The symmetry-adapted modeling is then achieved by expressing the Hamiltonian in terms of the linear combination of these bases belonging to the identity irreducible representation, and the model parameters (linear coefficients) in the Hamiltonian can be determined so as to reproduce the electronic structures given by the density-functional computation. We demonstrate our method for the modeling of graphene, and emphasize usefulness of the symmetry-adapted basis to analyze and predict physical phenomena and spontaneous symmetry breaking in a phase transition. The present method is complementary to de-facto standard Wannier tight-binding modeling, and it provides us with a fundamental basis to develop a symmetry-based analysis for materials science.

cond-mat.mtrl-sci↗