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Sang-Wook Cheong

Publications and source records attributed to Sang-Wook Cheong.

At least 19 recordsLinked to original sources

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

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

Giant spontaneous Kerr effect and its self-doping dependence in altermagnetic MnTe

Altermagnetism, a third class of collinear magnetism with spin-split bands and vanishing net magnetization, has emerged in hexagonal α-MnTe, a promising platform for ultrafast, stray-field-free spintronics. Whether MnTe's macroscopic symmetry-breaking signatures reflect ideal altermagnetic order or are activated by defects remains open. Here we report giant spontaneous Kerr rotations of up to 1500 rad in α-MnTe single crystals at the telecommunication wavelength of 1550 nm, onsetting precisely at the Néel temperature TN = 307 K. The signal appears in disjoint macroscopic patches whose amplitude tracks the sample conductivity, and a hole-conducting α-MnTe film reproduces this response together with an anomalous Hall effect. Within a single crystal, Kerr-active regions are optically distinct from their Kerr-silent surroundings in co-registered reflection maps. These observations indicate that carrier self-doping, rather than ideal altermagnetic order alone, governs the giant magneto-optical response, and establish telecom-wavelength Kerr imaging as a practical readout for altermagnetic spintronics.

cond-mat.str-el

Nonlinear Breakdown of Antisymmetric Flexoelectric Coupling

Flexoelectric coupling is conventionally regarded as antisymmetric, such that reversing the strain gradient reverses the polarization direction while preserving its magnitude. Here we report that this antisymmetric coupling breaks down in noncentrosymmetric single crystals driven by large strain gradients, where nonlinearity becomes operative. Harmonic-resolved measurements reveal robust even-order flexoelectric harmonics that are forbidden in antisymmetric systems, as well as the three-wave mixing indicative of symmetry breaking under dual-frequency excitation. These frequency-relevant generations provide evidence for asymmetric flexoelectricity in the nonlinear regime. A reconstructed nonlinear constitutive framework consistently accounts for all observations by incorporating even-order strain-gradient terms. Our findings establish asymmetric flexoelectricity as an intrinsic electromechanical response and uncover a symmetry-breaking mechanism in flexoelectricity.

cond-mat.mtrl-sci

X-ray magnetic circular dichroism evidence of intrinsic $d$-wave altermagnetism in rutile-structure NiF$_2$

We present the x-ray magnetic circular dichroism (XMCD) at the Ni $L_{2,3}$-edge as an evidence of the $d$-wave altermagnetism in rutile-structure NiF$_2$. Sizable XMCD signal is observed in excellent agreement with theoretical simulations. Owing to a considerable net magnetization due to spin canting, the XMCD spectrum consists of an altermagnetic signal as well as a non-negligible ferromagnetic contribution. We verify experimentally that the XMCD spectrum can be written as a sum of contributions from altermagnetism and weak ferromagnetism. Two experimental methods to isolate the ferromagnetic contribution are shown to yield essentially the same result. These are dependence of XMCD on applied magnetic fields below the Néel temperature and the XMCD measured in applied field above the Néel temperature. Our results demonstrate the utility of XMCD as a probe for altermagnetic materials with the coexisting weak ferromagnetism induced by the relativistic spin-orbit coupling.

cond-mat.str-el

Why are there so few non-altermagnetic antiferromagnets?

We review the conditions that cause or prohibit non-relativistic spin splitting of the energy bands in antiferromagnets. We propose that the existence of spin splitting in magnetically ordered systems is the default scenario and outline the criteria that must be met to avoid it. We discuss some of the properties of those special antiferromagnets that succeed in preserving their spin degeneracy.

cond-mat.mtrl-sci

Topological Magneto-optical Kerr Effect without Spin-orbit Coupling in Spin-compensated Antiferromagnet

The magneto-optical Kerr effect (MOKE), the differential reflection of oppositely circularly polarized light, has traditionally been associated with relativistic spin-orbit coupling (SOC), which links a particle's spin with its orbital motion. In ferromagnets, large MOKE signals arise from the combination of magnetization and SOC, while in certain coplanar antiferromagnets, SOC-induced Berry curvature enables MOKE despite zero net magnetization. Theoretically, large MOKE can also arise in a broader class of magnetic materials with compensated spins, without relying on SOC - for example, in systems exhibiting real-space scalar spin chirality. The experimental verification has remained elusive. Here, we demonstrate such a SOC- and magnetization-free MOKE in the noncoplanar antiferromagnet Co1/3TaS2. Using a Sagnac interferometer microscope, we image domains of scalar spin chirality and their reversal. Our findings establish experimentally a new mechanism for generating large MOKE signals and position chiral spin textures in compensated magnets as a compelling platform for ultrafast, stray-field-immune opto-spintronic applications.

physics.optics

Atomically-sharp magnetic soliton in the square-net lattice EuRhAl$_{4}$Si$_{2}$

Topological spin textures are hallmark manifestations of competing interactions in magnetic matter. Their effective description by nonlinear field theories reflects an energetic frustration that destabilizes uniform order while selecting finite-size, topologically nontrivial configurations as stationary states. Among the most extreme realizations are atomically-sharp domain wall excitations, namely one-dimensional (1D) magnetic solitons, which represent the ultimate scaling limit of magnetic textures. Such solitons may emerge in magnetic systems where effective exchange interactions compete directly with uniaxial magnetic anisotropy. Here we show that the square-net rare earth compound EuRhAl$_{4}$Si$_{2}$ realizes a very susceptible regime where the magnetic anisotropy competes with highly frustrated exchange interactions stabilizing a rare ferrimagnetic $\uparrow\uparrow\downarrow$ state that, under applied magnetic field, supports the formation of atomically-sharp soliton defects. We confirm the bulk response of the 1D magnetic solitons via magnetization and electrical transport measurements. We establish both the zero- and in-field $\uparrow\uparrow\downarrow$ order via neutron diffraction, while magnetic force microscopy visualizes its real-space evolution into a stripe-like array. To elucidate the microscopic origin of the soliton, we relate the Ruderman-Kittel-Kasuya-Yosida (RKKY)-driven exchange interactions and the magnetic anisotropy through density functional theory, and we construct an effective 1D $J_{1}$-$J_{2}$-$K$ model whose atomistic spin dynamics simulations reproduce the observed soliton states as a function of external field. Our results demonstrate that EuRhAl$_{4}$Si$_{2}$ hosts atomically-sharp, field-driven 1D magnetic solitons, providing a new platform for studying 1D topological excitations at the atomic length scale.

cond-mat.str-el

Anisotropic magnon transport in an antiferromagnetic trilayer heterostructure: is BiFeO$_3$ an altermagnet?

Magnons provide a route to ultra-fast transport and non-destructive readout of spin-based information transfer. Here, we report magnon transport and its emergent anisotropic nature in BiFeO$_3$ layers confined between ultrathin layers of the antiferromagnet LaFeO$_3$. Due to the confined state, BiFeO$_3$ serves as an efficient magnon transmission channel as well as a magnetoelectric knob by which to control the stack by means of an electric field. We discuss the mechanism of the anisotropic spin transport based on the interaction between the antiferromagnetic order and the electric field. This allows us to manipulate and amplify the spin transport in such a confined geometry. Furthermore, lower crystal symmetric and suppression of the spin cycloid in ultrathin BiFeO$_3$ stabilizes a non-trivial antiferromagnetic state exhibiting symmetry-protected spin-split bands that provide the non-trivial sign inversion of the spin current, which is a characteristic of an altermagnet. This work provides an understanding of the anisotropic spin transport in complex antiferromagnetic heterostructures where ferroelectricity and altermagnetism coexist, paving the way for a new route to realize electric-field control of a novel state of magnetism.

cond-mat.mes-hall

Spectroscopic Demarcation of Emergent Photons and Spinons in a Dipolar-Octupolar Quantum Spin Liquid

The identification of fractionalized excitations in quantum spin liquids (QSLs) remains a central challenge in condensed matter physics. In dipolar-octupolar (DO) pyrochlores, such as $\text{Ce}_2\text{Zr}_2\text{O}_7$, the candidate $π$-flux quantum spin ice (QSI) state is predicted to host both gapless emergent photons and a continuum of spinons. However, resolving these modes at zero field is complicated by their spectral overlap and the presence of nonmagnetic scattering near zero energy. Here, we report neutron scattering experiments on $\text{Ce}_2\text{Zr}_2\text{O}_7$ under a magnetic field along the $[1,1,1]$ direction. In contrast to previous unpolarized studies at zero-field that relied on high-temperature subtraction, we use a same-temperature high-field subtraction protocol to isolate the photon mode. Leveraging the selective coupling of the magnetic field to the dipolar degrees of freedom, we demonstrate the spectroscopic demarcation of these excitations. We observe that weak fields ($\approx 0.15$ T) suppress the low-energy photon weight while leaving the high-energy spinon continuum robust, albeit hardened. Our results, supported by gauge mean-field theory and exact diagonalization calculations, provide strong evidence for the $π$-flux QSI state and introduce a powerful field-tuning protocol for investigating DO-QSLs.

cond-mat.str-el

Polar enhancement of optical nonlinearities and domain-driven second harmonic contrast in bismuth telluro-halide van der Waals crystals

The BiTeX family of polar van der Waals (vdW) semiconductors offers a unique platform for exploring the interplay between polar crystalline structure and nonlinear optical phenomena. Here, we utilize second harmonic generation (SHG) polarimetry to demonstrate giant anisotropic optical nonlinearities in BiTeBr and BiTeI driven by contributions to the crystals' nonlinear polarizability originating from their permanent dipole moment. In addition, using SHG microscopy, we show that BiTeI displays a distinctive SHG spatial texture consisting of thread-like regions of reduced harmonic intensity. These features demark the boundaries between phase and anti-phase polar domains, confirmed via piezoresponse force microscopy and are attributable to disorder-driven restoration of inversion symmetry and concomitant optical interference effects. Our results unveil the power of polarization-resolved SHG microscopy in elucidating the intricate relationship between structure, symmetry, and nonlinear optical responses in polar vdW materials and highlight the promise of BiTeX as a material platform for domain-engineered nanoscale nonlinear photonics.

physics.optics

Yu-Shiba-Rusinov bound states of exciton condensate

Quantum condensed states in solids often reveal their fundamental nature via interactions with impurities, as epitomized by Yu-Shiba-Rusinov (YSR) bound states at magnetic impurities in superconductors. Although analogous YSR bound states were predicted within quantum condensates of excitons several decades ago, their existence has been elusive. Here, we directly visualize in-gap electronic states bound to impurities inside an exciton condensate phase of a van der Waals crystal Ta2Pd3Te5, utilizing scanning tunneling microscopy and spectroscopy. We find that the energies of in-gap states are strongly correlated with the excitonic band gap, which is systematically tuned by local strain and carrier injection. Our theoretical analyses reveal that these in-gap states are induced by charge dipoles associated with Ta vacancies through a charge-exciton version of the YSR mechanism. Our findings establish both the YSR physics in exciton condensates and a novel microscopic tool to probe and control quantum properties in exciton condensates persisting up to room temperature.

cond-mat.str-el

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

All-Electrical Self-Switching of van der Waals Chiral Antiferromagnet

Antiferromagnets have garnered significant attention due to their negligible stray field and ultrafast magnetic dynamics, which are promising for high-density and ultrafast spintronic applications. Their dual functionality as both spin sources and information carriers could enable all-electrical self-induced switching of antiferromagnetic order, offering great potential for ultra-compact spintronic devices. However, related progress is still elusive. Here, we report the deterministic switching of chiral antiferromagnetic orders induced by charge current at zero external magnetic field in the van der Waals (vdW) magnetically intercalated transition metal dichalcogenide CoTa3S6. This system exhibits strong interactions between cobalt atom magnetic moment lattice and itinerant electrons within the metallic layers, as demonstrated by temperature-dependent angle-resolved photoemission, scanning tunneling spectroscopy, and topological Nernst effect measurements. Notably, the itinerant-localization interactions lead to current-induced chiral spin orbit torques as well as Ruderman-Kittel-Kasuya-Yosida (RKKY) exchange torques that interact with the localized magnetic moments, facilitating all-electrical switching of the chiral magnetic order in the CoTa3S6 flake. Our work opens a promising avenue for manipulating antiferromagnetic orders by delicately engineering the synergistic interactions between magnetic moments and itinerant electrons.

cond-mat.mes-hall

Mesoscopic Helices of Polar Domains in a Quadruple Perovskite

A significant effort in condensed matter physics is dedicated to the search for exotic arrangements of electric dipoles in crystals. Non-collinear dipolar arrangements mimicking magnetic spin textures, such as polar vortices and skyrmions, have been realized, but others, like helices of dipoles, have remained elusive. While earlier work claimed the presence of a helical dipole modulation in ferroelectric BiCu$_{x}$Mn$_{7-x}$O$_{12}$, our results rule out such a structure, motivating a renewed search for helical textures. Using atomic-resolution imaging, we report a novel form of helical order in which polar domains self-organize into a mesoscopic helical pattern: from domain to domain, polarization rotation follows a consistent handedness. Both right- and left-handed chirality emerging from this helical ordering are observed. This discovery establishes mesoscopic ordering as novel mechanism for inducing helical textures, and hence chirality, in ferroelectric crystals, paralleling the efforts in liquid crystals and supramolecular assemblies.

cond-mat.mes-hall

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

Tuning Coupled Toroidic and Polar Orders in a Bilayer Antiferromagnet

Magnetic toroidal order features a loop-like arrangement of magnetic dipole moments, thus breaking both spatial inversion (P) and time-reversal (T) symmetries while preserving their combined PT sym-metry. This PT symmetry enables a linear magnetoelectric effect, allowing the coupling between magnetic toroidicity and electric polarity. However, the detection and control of two-dimensional (2D) magnetic toroidal order and the investigation of its linear magnetoelectric response remain largely unexplored. Here, using bilayer CrSBr as a platform, which hosts an in-plane layer-antiferromagnetic (AFM) order and simultaneously exhibits a magnetic toroidal order, we show compelling evidence for tuning this 2D magnetic toroidicity and its induced electric polarity through magnetic-field-depend-ent second harmonic generation (SHG). Under an out-of-plane magnetic field, we decompose the SHG signal into a time-reversal-odd component that scales with the magnetic toroidal moment and a time-reversal-even component that is proportional to the electric polarization. When sweeping the magnetic field from positive to negative values, we observe that the magnetic toroidicity retains its sign but diminishes in magnitude at higher fields while the electric polarity flips its sign and increases in strength at increasing fields below a critical threshold. When applying an in-plane electric field along the Néel vector direction, together with an out-of-plane field, we find that the magnetic toroidal and electric polar domains are moved in a locked fashion. These findings underscore the promise of 2D magnetic toroidal order in realizing giant linear magnetoelectric effects, opening exciting possi-bilities for next-generation electronic, magnetic, optical, and photonic devices enabled by 2D mag-netoelectrics.

cond-mat.mtrl-sci

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