arXiv subjects

Xianghan Xu

Publications and source records attributed to Xianghan Xu.

At least 19 recordsLinked to original sources

arXiv2026

Direct observation of phonon mode with an antisymmetric Raman tensor

Phonon angular momentum, characterized by circular or elliptical motion of atoms, plays a decisive role in diverse phenomena, ranging from the phonon Hall effect, phonon magnetic moment, Einstein-de Haas effect, Weyl phonons, and driven chiral phonons. The phonon modes with an antisymmetric Raman tensor, which carry an intrinsic phonon angular momentum in a pseudovector symmetry channel, have been overlooked in the past in the chiral phonon community. Here, we report the detection of this type of phonon mode using polarization-resolved Raman spectroscopy. We observe a phonon at 266cm$^{-1}$ in the antiferromagnetic chiral phase of Cr$_2$O$_3$ in the $A_2$-pseudovector symmetry channel. This $A_2$ mode's frequency and the elliptical motion are captured by first-principles phonon calculations, which treat both lattice and spins on an equal footing as 'slow' degrees of freedom. This mode gets Raman activity due to the presence of Cr vacancies in Cr$_2$O$_3$ that locally break the twofold rotational symmetry perpendicular to the threefold axis. Our results provide a new way to detect the novel symmetry-forbidden $A_2$ phonon modes with an antisymmetric Raman tensor in a pseudovector symmetry channel.

cond-mat.mtrl-sci↗

arXiv2026

Magnetic quantum defects in a uniaxial antiferromagnetic insulator

Point defects have been successfully utilized in various quantum technologies, serving as quantum qubits for quantum computation, single-photon emitters for quantum communication, and nanoscale sensors for quantum metrology. However, their further development faces key challenges, particularly in discovering and exploring suitable defect-host systems that meet the necessary criteria for quantum applications. Here, using polarization-resolved Raman spectroscopy and terahertz absorption spectroscopy, we discover three distinct chromium-vacancy-induced excitations in the uniaxial antiferromagnetic insulator, Cr$_2$O$_3$. These vacancy-induced excitations have an energy scale of a few tens of millielectronvolts and are twofold degenerate, and the lowest one at 64 $cm^{-1}$ is sharp and sensitive to the external magnetic field along the easy-axis direction, particularly close to the spin-flop regime around 6T, where the mode softens from 64 to 27$cm^{-1}$. Based on the defect supercell first-principles calculations, we interpret the mode at 64 $cm^{-1}$ as a local magnetic excitation of the local moment within the chromium vacancy state. Our results establish that the magnetic defect states in Cr$_2$O$_3$ have potential for quantum applications.

cond-mat.mtrl-sci↗

arXiv2026

Chirality Transfer to the Magnetic Sublattice in the Hybrid Perovskite (R)-/(S)-3-Fluoropyrrolidinium Copper(II) Chloride

Incorporating chiral organic cations into organic-inorganic hybrid materials has been shown to enable the inorganic sublattice to display chiroptical properties. We report a new two-dimensional magnetic ($S=1/2$) chiral metal halide perovskite, (R)- and (S)-$(C_4H_9FN)_2CuCl_4$ (where $(C_4H_9FN)^+$ is 3-fluoropyrrolidinium), which consists of Cu-Cl inorganic layers separated by $(C_4H_9FN)^+$ organic cations. The presence of the chiral $(C_4H_9FN)^+$ organic cation induces formation of chiral magnetic order, even though the inorganic sublattice itself is nearly structurally centrosymmetric. We also report the racemic variant, containing an equal amount of (R)- and (S)- cations, which shows no evidence of chiral magnetic order. When the magnetic susceptibility is measured perpendicular to inorganic Cu-Cl layer propagation direction, an antiferromagnetic phase transition at Néel temperature $T_N = 2.23~K$ is observed in both the chiral and racemic materials, and the existence of the magnetic phase transition is supported by specific heat capacity measurements. Field-induced magnetic chirality is observed through the existence of a second-order magnetoelectric effect in the chiral variant, while no magnetoelectric signal is observed for the racemic material, indicating the absence of magnetic chirality. Our findings demonstrate that materials exhibiting chiral magnetic order can be created through the incorporation of a chiral cation into an organic-inorganic hybrid magnetic material, potentially allowing for the design of tailored materials that combine chiral magnetism with other desirable optical and electronic properties that come from structural chirality.

cond-mat.mtrl-sci↗

arXiv2026

Crystal structure and basic properties of dirhenate quantum materials

The anhydrous divalent 3d-metal dirhenate quantum materials, M(ReO$_4$)$_2$,were synthesized using solid-state methods for M = Mn through Zn. Previously unreported Mg(ReO4)2 is also described. Their layered crystal structures, which feature an in-plane triangular lattice of M$^{2+}$, were refined using single crystal X-ray diffraction, and their optical absorption and several other physical properties were characterized. Their magnetism and heat capacity reveal long-range magnetic order at low temperatures in many of the M(ReO$_4$)$_2$ phases. Notably, many of these ordered states are sensitive to applied magnetic fields and can be readily suppressed by relatively small fields, suggesting competing magnetic interactions in a low-dimensional framework, which appear worthy of further study.

cond-mat.mtrl-sci↗

arXiv2026

Magnetization Plateaus in the Spin-Orbit Coupled Bilayer Triangular Lattice Antiferromagnet Rb2Co2(SeO3)3

Geometric frustration among competing spin exchanges can give rise to novel quantum phases by enhancing fluctuations that drive magnetic systems beyond the classical regime. We investigate the frustrated array of strongly correlated spin dimers in the bilayer triangular lattice antiferromagnet \rcs{} under applied magnetic fields. A cascade of magnetization plateaus appears at $M/M_s = 1/3, 1/2, 2/3,$ and $5/6$, together with a weak anomalous feature near $M/M_s = 1/6$, in fields up to 60 T. Concurrent changes in magneto-dielectric response follows the plateau boundaries. The finite slope of each plateau and the absence of a zero-field gap in our ultralow-temperature ac susceptibility down to 20 mK indicate broken $U(1)$ spin-rotation symmetry. A minimal bilayer-dimer model treated with bond operator representation reproduces the low-field sequence only when $U(1)$ symmetry is explicitly lifted by spin-orbit-driven, bond-dependent anisotropy. Near saturation, a projected triangular pseudospin model accounts for the high-field plateaus with modest further-neighbor interactions. These results demonstrate that anisotropic exchange arising from spin-orbit-coupled moments is essential for stabilizing the full plateau hierarchy in \rcs{}, a mechanism overlooked in previous interpretations of Co-based triangular bilayers.

cond-mat.str-el↗

arXiv2025

Nonreciprocal Transport in chiral Mo3Al2C Near the Superconducting to Normal Transition

We investigate nonreciprocal electrical transport in bulk single-crystalline Mo3Al2C, a material known to host crystallographic chirality, a polar charge-density-wave instability, and a superconducting transition near 8 K. Using AC transport measurements to analyze the first-harmonic and second-harmonic resistance responses, we observe a distinct nonreciprocal second-harmonic signal that is significantly enhanced near the boundary of the normal and superconducting phases. Phenomenologically, this response arises from direction-dependent coupling between the external magnetic field and the current-induced intrinsic magnetization within the chiral lattice. Furthermore, a persistent nonreciprocal response observed under perpendicular magnetic fields suggests a toroidal-induced effect linked to the electric polarization emerging from the charge-density-wave phase. These results demonstrate that bulk Mo3Al2C serves as an intrinsic platform for tunable nonreciprocal transport rooted in the interplay of chirality, polarity, and superconductivity.

cond-mat.supr-con↗

arXiv2025

Phase Diagram and Spectroscopic Signatures of a Supersolid in Quantum Ising Magnet K$_2$Co(SeO$_3$)$_2$

A supersolid is a quantum-entangled state of matter exhibiting the dual characteristics of superfluidity and solidity. Theory predicts that hard-core bosons with repulsive interactions on a triangular lattice can form supersolid phases at half filling and near complete filling. Leveraging an exact mapping between bosons and spin-$\frac{1}{2}$ degrees of freedom, we investigate these phases in the spin-$\frac{1}{2}$ triangular-lattice antiferromagnet \K212 with exchange constants $J_z = 2.96(2)$~meV and $J_{\perp} = 0.21(3)$~meV. At zero field, neutron diffraction reveals the gradual development for $T<15$~K of quasi-two-dimensional $\sqrt{3}\times\sqrt{3}$ magnetic order with $Z_3$ translational symmetry breaking (solidity) albeit with 44(5)% reduced amplitude at $T=0.3$~K indicating strong quantum fluctuations. These are apparent in equidistant bands of continuum neutron scattering for $\hslashω_n\approx n\times J_z$, where $n=0,1,2,3$. The lowest energy ($n=0$) $\bf Q$-dependent continuum has a lower resonant edge and includes a quasi-elastic component at K $(\frac{1}{3}\frac{1}{3})$ consistent with broken $U(1)$ spin rotational symmetry (boson superfluidity). Competing instabilities are apparent in soft albeit finite-energy modes at M $(\frac{1}{2}0)$ and at $\frac{1}{2}$K $(\frac{1}{6}\frac{1}{6})$. For $\bf c$-axis-oriented magnetic fields $17~{\rm T} <μ_0 H< 21~{\rm T}$ that almost saturate the magnetization, corresponding to nearly filling the lattice with bosons, we find a new phase consistent with a second supersolid. These phases are separated by a pronounced 1/3 magnetization plateau that supports coherent spin waves, from which we determine the spin Hamiltonian.

cond-mat.str-el↗

arXiv2025

Electrotoroidicity: New Paradigm for Transverse Electromagnetic Responses

The exploration of transverse electromagnetic responses in solids with broken spatial-inversion (I) and/or time-reversal (T) symmetries has unveiled numerous captivating phenomena, including the (anomalous) Hall effect, Faraday rotations, non-reciprocal directional dichroism, and off-diagonal linear magnetoelectricity, all within the framework of magnetotoroidicity. Here, we introduce a novel class of transverse electromagnetic responses originating from electrotoroidicity in ferro-rotational (FR) systems with preserved I and T symmetries, distinct from magnetotoroidicity. We discover a high-order off-diagonal magnetic susceptibility of FR domains and a reduced linear diagonal magnetic susceptibility at FR domain walls in doped ilmenite FeTiO3. The non-trivial "Hall-like" effect of the former corresponds to an anomalous transverse susceptibility in the presence of spontaneous electrotoroidal moments in FR materials. Our findings unveil an emergent type of transverse electromagnetic responses even in I and T symmetry-conserved conditions and illustrate new functionalities of abundant FR materials.

cond-mat.mtrl-sci↗

arXiv2025

Controlled growth of polar altermagnets via chemical vapor transport

Altermagnetic properties have been recently proposed in polar magnetic oxides, M$_{2}$Mo$_{3}$O$_{8}$ (M = Mn, Fe, Co, Ni), where improved characteristics of stronger magnetoelectric coupling and higher magnetic transition temperatures were observed. Thus, understanding their microscopic origins is of fundamental and technological importance. However, the difficulty in growing large single crystals hinders detailed experimental studies. Here, we report the successful growth of large single crystals of the pyroelectric antiferromagnet using two representative compounds, Fe$_{2}$Mo$_{3}$O$_{8}$ and NiZnMo$_{3}$O$_{8}$. Growth was optimized using various parameters, finding the transport agent density as a primary factor, which depends strongly on the position of the pellet, the starting powder form, and the volume of the ampule. We demonstrated a controlled growth method by manipulating the convection and diffusion kinetics. High-quality crystals were characterized by using single-crystal X-ray diffraction, Laue diffraction, magnetic susceptibility, and Raman spectroscopy. Manipulation of magnetic properties through nonmagnetic Zn doping was shown in NiZnMo$_{3}$O$_{8}$. Our results enable the detailed investigation and manipulation of their unconventional altermagnetic and multiferroic properties. This study provides crucial insight into the controlled growth of other functional quantum materials.

cond-mat.mtrl-sci↗

arXiv2025

Phonon anomalies within the polar charge density wave phase of the structurally chiral superconductor Mo$_3$Al$_2$C

We employ polarization-resolved Raman spectroscopy to study the lattice dynamics of the polar charge density wave phase of the superconductor Mo$_3$Al$_2$C with structural chirality. We show the phononic signatures of the charge density wave transition at $T^*$ = 155\,K in Mo$_3$Al$_2$C. The detailed temperature dependence of these phonon modes' frequency, half width at half maximum, and integrated area below $T^*$ reveal anomalies at an intermediate temperature $T' \sim$ 100\,K, especially for the low-energy modes at 130 and 180\,\cm-1. We discuss the origin of these phonon anomalies within the polar charge density wave phase of Mo$_3$Al$_2$C.

cond-mat.supr-con↗

arXiv2025

Quantum spin dynamics of the honeycomb magnet K$_2$Co$_2$TeO$_6$ in high magnetic fields

We present terahertz spectroscopic measurements of quantum spin dynamics in the honeycomb magnet K$_2$Co$_2$TeO$_6$ as a function of temperature, polarization and in an external magnetic field applied in the honeycomb plane. Magnetic excitations are resolved below the magnetic ordering temperature of $T_\text{N}$ = 12 K. In the applied magnetic field, we reveal characteristic field dependence not only for the magnetic excitations observed at zero field, but also a rich set of modes emerging in finite fields. The observed magnetic excitations exhibit clear dependence on the terahertz polarization, and characteristic features at field-induced phase transitions consistent with our high-field magnetization data. We cannot evidently resolve a continuumlike feature, even when the long-range magnetic order is presumably suppressed in the strong magnetic field, indicating that a Kitaev-type interaction, if existing, is subleading in this compound.

cond-mat.str-el↗

arXiv2024

Polar charge density wave in a superconductor with crystallographic chirality

Symmetry plays an important role in determining the physical properties in condensed matter physics, as the symmetry operations of any physical property must include the symmetry operations of the point group of the crystal. As a consequence, crystallographic polarity and chirality are expected to have an impact on the Cooper pairing in a superconductor. While superconductivity with crystallographic polarity and chirality have both been found in a few crystalline phases separately; however, their coexistence and material realizations have not been studied. Here, by utilizing transport, Raman scattering, and transmission electron microscopy, we unveil a unique realization of superconductivity in single-crystalline Mo3Al2C (superconducting Tc=8K) with a polar charge-density-wave phase and well-defined crystallographic chirality. We show that the intriguing charge density wave order leads to a noncentrosymmetric-nonpolar to polar transition below T*=155K via breaking both the translational and rotational symmetries. Superconductivity emerges in this polar and chiral crystal structure below Tc=8K. Our results establish that Mo3Al2C is a superconductor with crystallographic polarity and chirality simultaneously, and motivate future studies of unconventional superconductivity in this category.

cond-mat.supr-con↗

arXiv2024

Spin Excitation Continuum in the Exactly Solvable Triangular-Lattice Spin Liquid CeMgAl11O19

In magnetically ordered insulators, elementary quasiparticles manifest as spin waves - collective motions of localized magnetic moments propagating through the lattice - observed via inelastic neutron scattering. In effective spin-1/2 systems where geometric frustrations suppress static magnetic order, spin excitation continua can emerge, either from degenerate classical spin ground states or from entangled quantum spins characterized by emergent gauge fields and deconfined fractionalized excitations. Comparing the spin Hamiltonian with theoretical models can unveil the microscopic origins of these zero-field spin excitation continua. Here, we use neutron scattering to study spin excitations of the two-dimensional (2D) triangular-lattice effective spin-1/2 antiferromagnet CeMgAl11O19. Analyzing the spin waves in the field-polarized ferromagnetic state, we find that the spin Hamiltonian is close to an exactly solvable 2D triangular-lattice XXZ model, where degenerate 120$^\circ$ ordered ground states - umbrella states - develop in the zero temperature limit. We then find that the observed zero-field spin excitation continuum matches the calculated ensemble of spin waves from the umbrella state manifold, and thus conclude that CeMgAl11O19 is the first example of an exactly solvable spin liquid on a triangular lattice where the spin excitation continuum arises from the ground state degeneracy.

cond-mat.str-el↗

arXiv2024

Electrical switching of Ising-superconducting nonreciprocity for quantum neuronal transistor

Nonreciprocal quantum transport effect is mainly governed by the symmetry breaking of the material systems and is gaining extensive attention in condensed matter physics. Realizing electrical switching of the polarity of the nonreciprocal transport without external magnetic field is essential to the development of nonreciprocal quantum devices. However, electrical switching of superconducting nonreciprocity remains yet to be achieved. Here, we report the observation of field-free electrical switching of nonreciprocal Ising superconductivity in Fe3GeTe2/NbSe2 van der Waals (vdW) heterostructure. By taking advantage of this electrically switchable superconducting nonreciprocity, we demonstrate a proof-of-concept nonreciprocal quantum neuronal transistor, which allows for implementing the XOR logic gate and faithfully emulating biological functionality of a cortical neuron in the brain. Our work provides a promising pathway to realize field-free and electrically switchable nonreciprocity of quantum transport and demonstrate its potential in exploring neuromorphic quantum devices with both functionality and performance beyond the traditional devices.

cond-mat.mes-hall↗

arXiv2024

Interfacial magnetic spin Hall effect in van der Waals Fe3GeTe2/MoTe2 heterostructure

The spin Hall effect (SHE) allows efficient generation of spin polarization or spin current through charge current and plays a crucial role in the development of spintronics. While SHE typically occurs in non-magnetic materials and is time-reversal even, exploring time-reversal-odd (T-odd) SHE, which couples SHE to magnetization in ferromagnetic materials, offers a new charge-spin conversion mechanism with new functionalities. Here, we report the observation of giant T-odd SHE in Fe3GeTe2/MoTe2 van der Waals heterostructure, representing a previously unidentified interfacial magnetic spin Hall effect (interfacial-MSHE). Through rigorous symmetry analysis and theoretical calculations, we attribute the interfacial-MSHE to a symmetry-breaking induced spin current dipole at the vdW interface. Furthermore, we show that this linear effect can be used for implementing multiply-accumulate operations and binary convolutional neural networks with cascaded multi-terminal devices. Our findings uncover an interfacial T-odd charge-spin conversion mechanism with promising potential for energy-efficient in-memory computing.

cond-mat.mes-hall↗

arXiv2024

Symmetry breaking and ascending in the magnetic kagome metal FeGe

Spontaneous symmetry breaking-the phenomenon where an infinitesimal perturbation can cause the system to break the underlying symmetry-is a cornerstone concept in the understanding of interacting solid-state systems. In a typical series of temperature-driven phase transitions, higher temperature phases are more symmetric due to the stabilizing effect of entropy that becomes dominant as the temperature is increased. However, the opposite is rare but possible when there are multiple degrees of freedom in the system. Here, we present such an example of a symmetry-ascending phenomenon in a magnetic kagome metal FeGe by utilizing neutron Larmor diffraction and Raman spectroscopy. In the paramagnetic state at 460K, we confirm that the crystal structure is indeed hexagonal kagome lattice. On cooling to TN, the crystal structure changes from hexagonal to monoclinic with in-plane lattice distortions on the order of 10^(-4) and the associated splitting of the double degenerate phonon mode of the pristine kagome lattice. Upon further cooling to TCDW, the kagome lattice shows a small negative thermal expansion, and the crystal structure becomes more symmetric gradually upon further cooling. Increasing the crystalline symmetry upon cooling is unusual, it originates from an extremely weak structural instability that coexists and competes with the CDW and magnetic orders. These observations are against the expectations for a simple model with a single order parameter, hence can only be explained by a Landau free energy expansion that takes into account multiple lattice, charge, and spin degrees of freedom. Thus, the determination of the crystalline lattice symmetry as well as the unusual spin-lattice coupling is a first step towards understanding the rich electronic and magnetic properties of the system and sheds new light on intertwined orders where the lattice degree of freedom is no longer dominant.

cond-mat.str-el↗

arXiv2024

Giant X-ray circular dichroism in a time-reversal invariant altermagnet

X-ray circular dichroism, arising from the contrast in X-ray absorption between opposite photon helicities, serves as a spectroscopic tool to measure the magnetization of ferromagnetic materials and identify the handedness of chiral crystals. Antiferromagnets with crystallographic chirality typically lack X-ray magnetic circular dichroism because of time-reversal symmetry, yet exhibit weak X-ray natural circular dichroism. Here, we report the observation of giant natural circular dichroism in the Ni $L_3$-edge X-ray absorption of Ni$_3$TeO$_6$, a polar and chiral antiferromagnet with effective time-reversal symmetry. To unravel this intriguing phenomenon, we propose a phenomenological model that classifies the movement of photons in a chiral crystal within the same symmetry class as that of a magnetic field. The coupling of X-ray polarization with the induced magnetization yields giant X-ray natural circular dichroism, revealing the altermagnetism of Ni$_3$TeO$_6$. Our findings provide evidence for the interplay between magnetism and crystal chirality in natural optical activity. Additionally, we establish the first example of a new class of magnetic materials exhibiting circular dichroism with time-reversal symmetry.

cond-mat.str-el↗

arXiv2024

Ultrafast simultaneous manipulation of multiple ferroic orders through nonlinear phonon excitation

Recent experimental studies have demonstrated the possibility of utilizing strong terahertz pulses to manipulate individual ferroic orders on pico- and femtosecond timescales. Here, we extend these findings and showcase the simultaneous manipulation of multiple ferroic orders in BiFeO$_3$, a material that is both ferroelectric and antiferromagnetic at room temperature. We find a concurrent enhancement of ferroelectric and antiferromagnetic second-harmonic generation (SHG) following the resonant excitation of a high-frequency fully-symmetric phonon mode. Based on first-principles calculations and phenomenological modeling, we ascribe this observation to the inherent coupling of the two ferroic orders to the nonequilibrium distortions induced in the crystal lattice by nonlinearly driven phonons. Our finding highlights the potential of nonlinear phononics as a technique for manipulating multiple ferroic order parameters at once. In addition, this approach provides a promising avenue to studying the dynamical magnetization and polarization behavior, as well as their intrinsic coupling, on ultrashort timescales.

cond-mat.str-el↗