arXiv subjects

S. -W. Cheong

Publications and source records attributed to S. -W. Cheong.

At least 19 recordsLinked to original sources

arXiv2026

Highly controllable switching pathways in multiferroic GdMn$_2$O$_5$

Controlling magnetic moments using electric fields remains a central challenge in spintronics. Multiferroics, where magnetic and electric orders coexist, may be a natural platform for such control, but progress has been limited because interactions between these orders are typically too weak to overcome the energy barriers between magnetic states. A recently demonstrated topologically protected switching circumvents this limitation by exploiting reduced barriers at a phase transition. Nevertheless, the conditions enabling this phenomenon remain elusive and electric field control is poorly understood. Here, we experimentally map the energy landscape by tracking transitions in GdMn$_2$O$_5$ under combined electric and magnetic fields. The experiments reveal that the switching pathways can be controlled by the electric field. A minimal theoretical model captures the observed behavior, identifies the parameter space where switching paths are sensitive to small perturbations and reveals design principles for implementing topological switching in other materials.

cond-mat.mtrl-sci↗

arXiv2025

Critical Structural Parameter Determining Magnetic Phases in the Fe2Mo3O8 Altermagnet System

A systematic structural study of the Fe2Mo3O8 system as a function of pressure, temperature, and magnetic field reveals that the P63mc space group of this material remains stable for a broad range of these parameters. No changes are seen in the long-range structure for pressures between 0 and 10 GPa, temperatures between 11 K and 300 K, and magnetic fields up to 9 T. The magnetostructural response (delta c/c) for a magnetic field transverse to the c-axis displacement is determined. The system is found to exhibit strong magnetostructural coupling. The well-known magnetic-field-induced first-order transition is found to be isostructural, between two distinct altermagnet states, and is accessible by fields in the a-b plane. In terms of the c/a ratio, the structures between ambient pressure and 10 GPa are found to map onto the full Zn doping range ((Fe1-yZny)2Mo3O8,0<y<1) in this system. The results show that the critical sensitive structural parameter for tuning the magnetic properties with pressure, temperature, and pressure is the c-axis length. The results indicate that the magnetic order in this complex metal oxide system (A2Mo3O8, A=Co, Mn, and Ni) can be cleanly tuned by pressure, making this class of materials an excellent platform for magnetic order switching in films grown on piezoelectric substrates.

cond-mat.mtrl-sci↗

arXiv2025

Altermagnetism in 6H perovskites

The combination of a centrosymmetric crystallographic structure with local structural alternations and collinear antiferromagnetism can lead to broken PT (Parity $\times$ Time-reversal) symmetry, resulting in altermagnets with non-relativistic spin-split bands. The 6H perovskites with composition A$_3$BB'$_2$O$_9$ exhibit unique layered structural alternations and typically adopt an antiferromagnetic ground state. Here, we report the discovery that several 6H perovskites are indeed altermagnets exhibiting non-relativistic spin-split bands. We also explore the possible presence of net magnetization due to spin-orbit coupling in these materials, as well as the manifestation of giant piezomagnetism. Since the single crystals of 6H perovskites can be readily grown and cleavable, our findings provide a new avenue to study the cleaved atomically-flat surfaces of altermagnets with advanced experimental techniques such as spin-resolved scanning tunneling microscopy (STM) or spin-resolved angle-resolved photoemission spectroscopy (ARPES) to explore their spin splitting nature.

cond-mat.mtrl-sci↗

arXiv2025

Large magnon dichroism and other optical properties of hexagonal ferrite h-Lu0.6Sc0.4FeO3 with altermagnetic A2 spin ordering

Multiferroic hexagonal h-Lu0.6Sc0.4FeO3 single crystals with non-collinear spins were studied using the THz and Raman scattering spectroscopies and ellipsometry. Antiferromagnetic resonances, or magnons, were found at about 0.85 THz and 1.2 THz. These magnons harden as temperature increases and disappear above 130 K. This behavior is consistent with the magnetic susceptibility and a phase transition to a previously reported weak ferromagnetic state. A strong dichroism at the resonance with the AFM doublet has been observed at zero external magnetic field using both conventional circular polarization and THz vector vortex beams. This observation is attributed to the strong altermagnetic properties of h-Lu0.6Sc0.4FeO3 with a broken PT symmetry. The splitting of the magnon doublet in an external magnetic field applied long the c axis yields a g-factor of 3.0 for the Fe3+ ions. Raman spectra of the optical phonons revealed a Fano-type asymmetry due to their interaction with a continuum of polar excitations. Electronic transitions were studied with ellipsometry and the results were compared with the modelled using DFT+eDMFT.

cond-mat.other↗

arXiv2024

Surface Magnetism in Fe$_3$GeTe$_2$ Crystals

The surface magnetization of Fe$_3$GeTe$_2$ was examined by low-energy electron microscopy (LEEM) using an off-normal incidence electron beam. We found that the 180$^o$ domain walls are of Bloch type. Temperature-dependent LEEM measurements yield a surface magnetization with a surface critical exponent $β$1 = 0.79 +/- 0.02. This result is consistent with surface magnetism in the 3D semi-infinite Heisenberg ($β$1 = 0.84 +/- 0.01) or Ising ($β$1 = 0.78 +/- 0.02) models, which is distinctly different from the bulk exponent ($β$ = 0.34 +/- 0.07). The measurements reveal the power of LEEM with a tilted beam to determine magnetic domain structure in quantum materials. Single crystal diffraction measurements reveal inversion symmetry-breaking weak peaks and yield space group P-6m2. This Fe site defect-derived loss of inversion symmetry enables the formation of skyrmions in this Fe$_3$GeTe$_2$ crystal.

cond-mat.mtrl-sci↗

arXiv2024

Spin-Mediated Direct Photon Scattering by Plasmons in BiTeI

We use polarization resolved Raman spectroscopy to demonstrate that for a 3D giant Rashba system the bulk plasmon collective mode can directly couple to the Raman response even in the long wavelength $\mathbf q \rightarrow 0$ limit. Although conventional theory predicts the plasmon spectral weight to be suppressed as the square of its quasi-momentum and thus negligibly weak in the Raman spectra, we observe a sharp in-gap plasmon mode in the Raman spectrum of BiTeI below the Rashba continuum. This coupling, in a polar system with spin-orbit coupling, occurs without assistance from phonons when the incoming photon excitation is resonant with Rashba-split intermediate states. We discuss the distinctive features of BiTeI's giant Rashba system band structure that enable the direct observation of plasmon in Raman scattering.

cond-mat.str-el↗

arXiv2024

Electronic and Vibrational Excitations on the Surface of the Three-Dimensional Topological Insulator Bi$_2$Te$_{3-x}$Se$_{x}$ (x = 0, 2, 3)

We study surface states in the three-dimensional topological insulators Bi$_2$Te$_{3-x}$Se$_{x}$ (x = 0, 2, 3) by polarization resolved resonant Raman spectroscopy. By tracking the spectral intensity of the surface phonon modes with respect to the incident photon energy, we show that the surface phonons are qualitatively similar to their bulk counterparts. Using the resonant Raman excitation profile, we estimated the binding energy of the surface conduction bands relative to bulk conduction bands. In addition, we selectively excite the surface-to-bulk electronic continuum near the Fermi energy in Bi$_2$Se$_3$ to determine the strength of Fano interaction between the most prominent surface phonon and the surface-to-bulk continuum.

cond-mat.mtrl-sci↗

arXiv2023

Giant natural optical rotation from chiral electromagnons in a collinear antiferromagnet

In NiTe$_3$O$_6$ with a chiral crystal structure, we report on a giant natural optical rotation of the lowest-energy magnon. This polarization rotation, as large as 140 deg/mm, corresponds to a path difference between right and left circular polarizations that is comparable to the sample thickness. Natural optical rotation, being a measure of structural chirality, is highly unusual for long-wavelength magnons. The collinear antiferromagnetic order of NiTe$_3$O$_6$ makes this giant effect even more peculiar: Chirality of the crystal structure does not affect the magnetic ground state but is strongly manifested in the lowest excited state. We show that the dynamic magnetoelectric effect, turning this magnon to a magnetic- and electric-dipole active hybrid mode, generates the giant natural optical rotation. In finite magnetic fields, it also leads to a strong optical magnetochiral effect.

cond-mat.str-el↗

arXiv2023

Neutron scattering sum rules, symmetric exchanges, and helicoidal magnetism in MnSb$_2$O$_6$

MnSb$_{2}$O$_{6}$ is based on the noncentrosymmetric $P321$ space group with magnetic Mn$^{2+}$ ($S={5/2}$, $L\approx 0$) spins ordering below $T_{\mathrm{N}}=12$ K in a helicoidal structure. The ground state magnetic structure, expected to be built and originate from 7 Heisenberg exchange constants, has been shown to be coupled to the underlying crystallographic chirality with polar domain switching being reported. We apply neutron spectroscopy to extract these symmetric exchange constants. Given the high complexity of the magnetic exchange network, crystallographic structure and complications fitting linear spin-wave models, we take advantage of multiplexed neutron instrumentation to use the first moment sum rule of neutron scattering to estimate the 7 exchange constants. We then use these parameters to calculate the low-energy spin-waves in the Néel state to reproduce the neutron response without strong antisymmetric coupling. Using Green's response functions, the stability of long-wavelength excitations in the context of proposed magnetic structures is then discussed. The results show the presence of strong exchange constants for the chiral exchange pathways and illustrate an underlying coupling between crystallographic and magnetic ``chirality" through predominantely symmetric exchange.

cond-mat.str-el↗

arXiv2023

Spin-phonon interactions and magnetoelectric coupling in Co$_4$$B_2$O$_9$ ($B$ = Nb, Ta)

In order to explore the consequences of spin-orbit coupling on spin-phonon interactions in a set of chemically-similar mixed metal oxides, we measured the infrared vibrational properties of Co$_4B_2$O$_9$ ($B$ = Nb, Ta) as a function of temperature and compared our findings with lattice dynamics calculations and several different models of spin-phonon coupling. Frequency vs. temperature trends for the Co$^{2+}$ shearing mode near 150 cm$^{-1}$ reveal significant shifts across the magnetic ordering temperature that are especially large in relative terms. Bringing these results together and accounting for noncollinearity, we obtain spin-phonon coupling constants of -3.4 and -4.3 cm$^{-1}$ for Co$_4$Nb$_2$O$_9$ and the Ta analog, respectively. Analysis reveals that these coupling constants derive from interlayer (rather than intralayer) exchange interactions and that the interlayer interactions contain competing antiferromagnetic and ferromagnetic contributions. At the same time, beyond-Heisenberg terms are minimized due to fortuitous symmetry considerations, different than most other 4$d$- and 5$d$-containing oxides. Comparison with other contemporary oxides shows that spin-phonon coupling in this family of materials is among the strongest ever reported, suggesting an origin for magnetoelectric coupling.

cond-mat.mtrl-sci↗

arXiv2022

Free Electrons Holes and Novel Surface Polar Order in Tetragonal BaTiO3 Ground States

We find novel polar orders that yield electron (e-) and hole (h+) gas and depend on surface terminations, using density functional theory (DFT) that, unlike existing reports, relaxed all the ion positions of ATiO3 having spontaneous polarization Ps (A: alkali earth metal). By the experiments of atomic-oxygen cleaned surfaces of BaTiO3, we find both e- and h+ gas that are proven to originate from Ps and constrain electrostatic potential, which has been missing. These experiments that remarkably agree with the DFTs of defect free BaTiO3 reveal the properties of Ps-originated e-h+ and, for ferroelectric basics, an e-h+-posed intrinsic constraint on depolarization field arising from Ps in proper time ranges.

cond-mat.mtrl-sci↗

arXiv2022

Neutron diffraction in MnSb2O6: Magnetic and structural domains in a helicoidal polar magnet with coupled chiralities

MnSb$_{2}$O$_{6}$ is based on the structural chiral $P$321 space group #150 where the magnetic Mn$^{2+}$ moments ($S=5/2$, $L\approx 0$) order antiferromagnetically at $T_\mathrm{N}=12$ K. Unlike the related iron based langasite (Ba$_3$NbFe$_3$Si$_2$O$_{14}$) where the low temperature magnetism is based on a proper helix characterized by a time-even pseudoscalar `magnetic' chirality, the Mn$^{2+}$ ions in MnSb$_{2}$O$_{6}$ order with a cycloidal structure at low temperatures, described instead by a time-even vector `magnetic' polarity. A tilted cycloidal structure has been found [M. Kinoshita et al. Phys. Rev. Lett. 117, 047201 (2016)] to facilitate ferroelectric switching under an applied magnetic field. In this work, we apply polarized and unpolarized neutron diffraction analyzing the magnetic and nuclear structures in MnSb$_{2}$O$_{6}$ with the aim of understanding this magnetoelectric coupling. We find no evidence for a helicoidal magnetic structure with one of the spin envelope axes tilted away from the cycloidal $c$-axis. However, on application of a magnetic field $\parallel$ $\vec{c}$ the spin rotation plane can be tilted, giving rise to a cycloid-helix admixture that evolves towards a distorted helix (zero cycloidal component) for fields great than $\approx$ 2 T. We propose a mechanism for the previously reported ferroelectric switching based on coupled structural and magnetic chiralities requiring only an imbalance of structural chiral domains.

cond-mat.str-el↗

arXiv2022

Chiral Electronic Excitations in a Quasi-2D Rashba System BiTeI

The optical transitions between spin-polarized bands of the quasi-two dimensional Rashba system BiTeI are investigated using polarization resolved resonant Raman spectroscopy. We detect chiral excitations between states with opposite helicity and compare spectra to calculations within a three-band model. Using the resonant Raman excitation profile, we deduce the Rashba parameters and band gaps of the higher conduction bands near the Fermi level, and compare the parameters to values obtained by ab initio density function theory (DFT).

cond-mat.str-el↗

arXiv2022

Nonreciprocal directional dichroism at telecom wavelengths

Magnetoelectrics with ultra-low symmetry and spin-orbit coupling are well known to display a number of remarkable properties including nonreciprocal directional dichroism. As a polar and chiral magnet, Ni$_3$TeO$_6$ is predicted to host this effect in three fundamentally different configurations, although only two have been experimentally verified. Inspired by the opportunity to unravel the structure-property relations of such a unique light-matter interaction, we combined magneto-optical spectroscopy and first-principles calculations to reveal nonreciprocity in the toroidal geometry and compared our findings with the chiral configurations. We find that formation of Ni toroidal moments is responsible for the largest effects near 1.1 eV - a tendency that is captured by our microscopic model and computational implementation. At the same time, we demonstrate deterministic control of nonreciprocal directional dichroism in Ni$_3$TeO$_6$ across the entire telecom wavelength range. This discovery will accelerate the development of photonics applications that take advantage of unusual symmetry characteristics.

cond-mat.mtrl-sci↗

arXiv2022

Band-Mott mixing hybridizes the gap in Fe$_2$Mo$_3$O$_8$

We combined optical spectroscopy and first principles electronic structure calculations to reveal the charge gap in the polar magnet Fe$_2$Mo$_3$O$_8$. Iron occupation on the octahedral site draws the gap strongly downward compared to the Zn parent compound, and subsequent occupation of the tetrahedral site creates a narrow resonance near the Fermi energy that draws the gap downward even further. This resonance is a many-body effect that emanates from a flat valence band in a Mott-like state due to screening of the local moment - similar to expectations for a Zhang-Rice singlet, except that here, it appears in a semi-conductor. We discuss the unusual hybridization in terms of orbital occupation and character as well as the structure-property relationships that can be unveiled in various metal-substituted systems (Ni, Mn, Co, Zn).

cond-mat.str-el↗

arXiv2021

Metastable antiphase boundary ordering in CaFe$_{2}$O$_{4}$

CaFe$_{2}$O$_{4}$ is an $S=5/2$ antiferromagnet exhibiting two magnetic orders which shows regions of coexistence at some temperatures. Using a Green's function formalism, we model neutron scattering data of the spin wave excitations in this material, ellucidating the microscopic spin Hamiltonian. In doing so, we suggest that the low temperature A phase order $(\uparrow\uparrow\downarrow\downarrow)$ finds its origins in the freezing of antiphase boundaries created by thermal fluctuations in a parent B phase order $(\uparrow\downarrow\uparrow\downarrow)$. The low temperature magnetic order observed in CaFe$_{2}$O$_{4}$ is thus the result of a competition between the exchange coupling along $c$, which favors the B phase, and the single-ion anisotropy which stabilizes thermally-generated antiphase boundaries, leading to static metastable A phase order at low temperatures.

cond-mat.str-el↗

arXiv2021

Magnetic anisotropy of the van der Waals ferromagnet Cr$_2$Ge$_2$Te$_6$ studied by angular-dependent XMCD

The van der Waals ferromagnet Cr$_2$Ge$_2$Te$_6$ (CGT) has a two-dimensional crystal structure where each layer is stacked through van der Waals force. We have investigated the nature of the ferromagnetism and the weak perpendicular magnetic anisotropy (PMA) of CGT by means of X-ray absorption spectroscopy and X-ray magnetic circular dichroism (XMCD) studies of CGT single crystals. The XMCD spectra at the Cr $L_{2,3}$ edge for different magnetic field directions were analyzed on the basis of the cluster-model multiplet calculation. The Cr valence is confirmed to be 3+ and the orbital magnetic moment is found to be nearly quenched, as expected for the high-spin $t_{2g}$$^3$ configuration of the Cr$^{3+}$ ion. A large ($\sim 0.2$ eV) trigonal crystal-field splitting of the $t_{2g}$ level caused by the distortion of the CrTe$_6$ octahedron has been revealed, while the single-ion anisotropy (SIA) of the Cr atom is found to have a sign {\it opposite} to the observed PMA and too weak compared to the reported anisotropy energy. The present result suggests that anisotropic exchange coupling between the Cr atoms through the ligand Te $5p$ orbitals having strong spin-orbit coupling has to be invoked to explain the weak PMA of CGT, as in the case of the strong PMA of CrI$_3$.

cond-mat.mtrl-sci↗

arXiv2021

Spin texture induced by non-magnetic doping and spin dynamics in 2D triangular lattice antiferromagnet h-Y(Mn,Al)O3

Novel effects induced by nonmagnetic impurities in frustrated magnets and quantum spin liquid represent a highly nontrivial and interesting problem. A theoretical proposal of extended modulated spin structures induced by doping of such magnets, distinct from the well-known skyrmions has attracted significant interest. Here, we demonstrate that nonmagnetic impurities can produce such extended spin structures in h-YMnO3, a triangular antiferromagnet with noncollinear magnetic order. Using inelastic neutron scattering (INS), we measured the full dynamical structure factor in Al-doped h-YMnO3 and confirmed the presence of magnon damping with a clear momentum dependence. Our theoretical calculations can reproduce the key features of the INS data, supporting the formation of the proposed spin textures. As such, our study provides the first experimental confirmation of the impurity-induced spin textures. It offers new insights and understanding of the impurity effects in a broad class of noncollinear magnetic systems.

cond-mat.str-el↗