arXiv subjects

S. -W. Cheong

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

At least 37 records · Page 2Linked to original sources

arXiv2021

Total angular momentum dichroism of the terahertz vortex beams at the antiferromagnetic resonances

Terahertz vortex beams with different superposition of the orbital angular momentum $l={\pm}1$, ${\pm}2$, ${\pm}3$, and ${\pm}4$ and spin angular momentum $σ={\pm}1$ were used to study antiferromagnetic (AFM) resonances in TbFe$_3$(BO$_3$)$_4$ and Ni$_3$TeO$_6$ single crystals. In both materials we observed a strong vortex beam dichroism for the AFM resonances that are split in external magnetic field. The magnitude of the vortex dichroism is comparable to that for conventional circular dichroism due to $σ$. The selection rules at the AFM resonances are governed by the total angular momentum of the vortex beam: $j=σ+l$. In particular, for $l={\pm}2$, ${\pm}3$, and ${\pm}4$ the sign of $l$ is shown to dominate over that for conventional circular polarization $σ$.

cond-mat.str-el↗

arXiv2021

From one- to two-magnon excitations in the S=3/2 magnet $β$-CaCr$_2$O$_4$

We apply neutron spectroscopy to measure the magnetic dynamics in the S=3/2 magnet $β$-CaCr$_2$O$_4$ (T$_N$=21 K). The low-energy fluctuations, in the ordered state, resemble large-S linear spin-waves from the incommensurate ground state. However, at higher energy transfers, these semi-classical and harmonic dynamics are replaced by an energy and momentum broadened continuum of excitations. Applying kinematic constraints required for energy and momentum conservation, sum rules of neutron scattering, and comparison against exact diagonalization calculations, we show that the dynamics at high-energy transfers resemble low-S one-dimensional quantum fluctuations. $β$-CaCr$_2$O$_4$ represents an example of a magnet at the border between classical Néel and quantum phases, displaying dual characteristics.

cond-mat.str-el↗

arXiv2020

Imitation of spin density wave order in Cu$_3$Nb$_2$O$_8$

Spin density waves, based on modulated local moments, are usually associated with metallic materials, but have recently been reported in insulators which display coupled magnetic and structural order parameters. We discuss one such example, the multiferroic Cu$_3$Nb$_2$O$_8$, which is reported to undergo two magnetic phase transitions, first to a spin density wave phase at $T_N \approx 26.5K$, and then to a helicoidal structure coupled to an electric polarization below $T_2 \approx 24K$ [R. D. Johnson, et al., Phys. Rev. Lett., 107, 137205 (2011)] which breaks the crystallographic inversion symmetry. We apply spherical polarimetry to confirm the low-temperature magnetic structure, yet only observe a single magnetic phase transition to helicoidal order. We argue that the reported spin density wave originates from a decoupling of the components of the magnetic order parameter, as allowed by symmetry and driven by thermal fluctuations. This provides a mechanism for the magnetic, but not nuclear, structure to break inversion symmetry thereby creating an intermediate phase where the structure imitates a spin density wave. As the temperature is reduced, this intermediate structure destabilizes the crystal such that a structural chirality is induced, as reflected by the emergence of the electric polarization, and the imitation spin density wave relaxes into a generic helicoid. This provides a situation where the magnetic structure breaks inversion symmetry while the crystal structure remains centrosymmetric.

cond-mat.mtrl-sci↗

arXiv2020

Non-linear soliton confinement in weakly coupled antiferromagnetic spin chains

We analyze the low-energy dynamics of quasi one dimensional, large-$S$ quantum antiferromagnets with easy-axis anisotropy, using a semi-classical non-linear sigma model. The saddle point approximation leads to a sine Gordon equation which supports soliton solutions. These correspond to the movement of spatially extended domain walls. Long-range magnetic order is a consequence of a weak inter-chain coupling. Below the ordering temperature, the coupling to nearby chains leads to an energy cost associated with the separation of two domain walls. From the kink-antikink two-soliton solution, we compute the effective confinement potential. At distances large compared to the size of the solitons the potential is linear, as expected for point-like domain walls. At small distances the gradual annihilation of the solitons weakens the effective attraction and renders the potential quadratic. From numerically solving the effective one dimensional Schröedinger equation with this non-linear confinement potential we compute the soliton bound state spectrum. We apply the theory to CaFe$_{2}$O$_{4}$, an anisotropic $S=5/2$ magnet based upon antiferromagnetic zig-zag chains. Using inelastic neutron scattering, we are able to resolve seven discrete energy levels for spectra recorded slightly below the Néel temperature $T_\textrm{N}\approx 200$~K. These modes are well described by our non-linear confinement model in the regime of large spatially extended solitons.

cond-mat.str-el↗

arXiv2019

Infrared nano-spectroscopy of ferroelastic domain walls in hybrid improper ferroelectric Ca$_3$Ti$_2$O$_7$

Ferroic materials are well known to exhibit heterogeneity in the form of domain walls. Understanding the properties of these boundaries is crucial for controlling functionality with external stimuli and for realizing their potential for ultra-low power memory and logic devices as well as novel computing architectures. In this work, we employ synchrotron-based near-field infrared nano-spectroscopy to reveal the vibrational properties of ferroelastic (90$^\circ$ ferroelectric) domain walls in the hybrid improper ferroelectric Ca$_3$Ti$_2$O$_7$. By locally mapping the Ti-O stretching and Ti-O-Ti bending modes, we reveal how structural order parameters rotate across a wall. Thus, we link observed near-field amplitude changes to underlying structural modulations and test ferroelectric switching models against real space measurements of local structure. This initiative opens the door to broadband infrared nano-imaging of heterogeneity in ferroics.

cond-mat.mtrl-sci↗

arXiv2019

Spin-wave directional anisotropies in antiferromagnetic Ba$_{3}$NbFe$_{3}$Si$_{2}$O$_{14}$

Ba$_{3}$NbFe$_{3}$Si$_{2}$O$_{14}$ (langasite) is structurally and magnetically single domain chiral with the magnetic helicity induced through competing symmetric exchange interactions. Using neutron scattering, we show that the spin-waves in antiferromagnetic langasite display directional anisotropy. On applying a time reversal symmetry breaking magnetic field along the $c$-axis, the spin wave energies differ when the sign is reversed for either the momentum transfer $\pm$ $\vec{Q}$ or applied magnetic field $\pm$ $μ_{0}$H. When the field is applied within the crystallographic $ab$-plane, the spin wave dispersion is directionally \textit{isotropic} and symmetric in $\pm$ $μ_{0}$H. However, a directional anisotropy is observed in the spin wave intensity. We discuss this directional anisotropy in the dispersion in langasite in terms of a field induced precession of the dynamic unit cell staggered magnetization. Directional anisotropy, or often referred to as non reciprocal responses, can occur in antiferromagnetic phases in the absence of the Dzyaloshinskii-Moriya interaction or other effects resulting from spin-orbit coupling.

cond-mat.mtrl-sci↗

arXiv2019

Spectroscopic and first principle DFT+eDMFT study of complex structural, electronic, and vibrational properties of $M_2$Mo$_3$O$_8$ ($M$=Fe, Mn) polar magnets

Optical spectroscopy, X-ray diffraction measurements, density functional theory (DFT) and density functional theory + embedded dynamical mean field theory (DFT+eDMFT) have been used to characterize structural and electronic properties of hexagonal $M_2$Mo$_3$O$_8$ ($M$=Fe, Mn) polar magnets. Our experimental data are consistent with the room temperature structure belonging to the space group P6$_3$mc for both compounds. The experimental structural and electronic properties at room temperature are well reproduced within DFT+eDMFT method, thus establishing its predictive power in the paramagnetic phase. With decreasing temperature, both compounds undergo a magnetic phase transition and we argue that this transition is concurrent with a structural phase transition (symmetry change from P6$_3$mc) in the Fe compound and an isostructural transition (no symmetry change from P6$_3$mc) in the Mn compound. In addition, the unusual temperature dependent behavior of electronic d-d transitions in Fe$^{2+}$ ions is discussed.

cond-mat.str-el↗

arXiv2019

Spin-Liquid-Like State in Pure and Mn-Doped TbInO3 with Nearly Triangular Lattice

Inelastic neutron scattering studies in single crystals of TbInO3 and TbIn0.95Mn0.05O3 with nearly-triangular antiferromagnetic lattice are reported. At low energies, a broad and apparently gapless continuum of magnetic excitations, located at the triangular lattice (TL) Brillouin zone boundary, is observed. The data are well described by the uncorrelated nearest-neighbor valence bonds model. At higher energies, a broad excitation branch dispersing from the TL zone boundary is observed. No signs of static magnetic order are found down to the temperatures two orders of magnitude smaller than the effective interaction energy. The fluctuating magnetic moment exceeds two thirds of the Tb3+ free-ion value and is confined to the TL plane. These observations are consistent with a TL-based spin liquid state in TbInO3.

cond-mat.str-el↗

arXiv2019

Nature of the Structural Symmetries Associated with Hybrid Improper Ferroelectricity in Ca3X2O7

In hybrid improper ferroelectric systems, polarization arises from the onset of successive nonpolar lattice modes. In this work, measurements and modeling were performed to determine the spatial symmetries of the phases involved in the transitions to these modes. Structural and optical measurements reveal that the tilt and rotation distortions of the MnO6 or TiO6 polyhedra relative to the high symmetry phases driving ferroelectricity in the hybrid improper Ca3X2O7 system (X=Mn and Ti) condense at different temperatures. The tilt angle vanishes abruptly at T$_T$ ~ 400 K for Ca3Mn2O7 (and continuously for X=Ti) and the rotation mode amplitude is suppressed at much higher temperatures T$_R$ ~1060 K. Moreover, Raman measurements in Ca3Mn2O7 under isotropic pressure reveal that the polyhedral tilts can be suppressed by very low pressures (between 1.4 and2.3 GPa) indicating their softness. These results indicate that the Ca3Mn2O7 system provides a new platform for strain engineering of ferroelectric properties in film based systems with substrate induced strain.

cond-mat.mtrl-sci↗

arXiv2019

Observation of Chiral Surface Excitons in a Topological Insulator Bi$_2$Se$_3$

The protected electron states at the boundaries or on the surfaces of topological insulators (TIs) have been the subject of intense theoretical and experimental investigations. Such states are enforced by very strong spin-orbit interaction in solids composed of heavy elements. Here, we study the composite particles -- chiral excitons -- formed by the Coulomb attraction between electrons and holes residing on the surface of an archetypical three-dimensional topological insulator (TI), Bi$_2$Se$_3$. Photoluminescence (PL) emission arising due to recombination of excitons in conventional semiconductors is usually unpolarized because of scattering by phonons and other degrees of freedom during exciton thermalization. On the contrary, we observe almost perfectly polarization-preserving PL emission from chiral excitons. We demonstrate that the chiral excitons can be optically oriented with circularly polarized light in a broad range of excitation energies, even when the latter deviate from the (apparent) optical band gap by hundreds of meVs, and that the orientation remains preserved even at room temperature. Based on the dependences of the PL spectra on the energy and polarization of incident photons, we propose that chiral excitons are made from massive holes and massless (Dirac) electrons, both with chiral spin textures enforced by strong spin-orbit coupling. A theoretical model based on such proposal describes quantitatively the experimental observations. The optical orientation of composite particles, the chiral excitons, emerges as a general result of strong spin-orbit coupling in a 2D electron system. Our findings can potentially expand applications of TIs in photonics and optoelectronics.

cond-mat.mes-hall↗

arXiv2018

Imaging antiferromagnetic antiphase domain boundaries using magnetic Bragg diffraction phase contrast

Manipulating magnetic domains is essential for many technological applications. Recent breakthroughs in Antiferromagnetic Spintronics brought up novel concepts for electronic device development. Imaging antiferromagnetic domains is of key importance to this field. Unfortunately, some of the basic domain types, such as antiphase domains, cannot be imaged by conventional techniques. Herein, we present a new domain projection imaging technique based on the localization of domain boundaries by resonant magnetic diffraction of coherent x rays. Contrast arises from reduction of the scattered intensity at the domain boundaries due to destructive interference effects. We demonstrate this approach by imaging antiphase domains in a collinear antiferromagnet Fe2Mo3O8, and observe evidence of domain wall interaction with a structural defect. This technique does not involve any numerical algorithms. It is fast, sensitive, produces large-scale images in a single-exposure measurement, and is applicable to a variety of magnetic domain types.

cond-mat.mes-hall↗

arXiv2018

Magnetic excitations in bulk multiferroic two-dimensional triangular lattice antiferromagnet (Lu,Sc)FeO$_3$

Non-collinear two-dimensional triangular lattice antiferromagnets (2D TLAF) are currently an area of very active research due to their unique magnetic properties, which lead to non-trivial quantum effects that experimentally manifest themselves in the spin excitation spectra. Recent examples of such insulating 2D TLAF include (Y,Lu)MnO$_3$, LiCrO$_2$, and CuCrO$_2$. Hexagonal LuFeO3 is a recently synthesized 2D TLAF which exhibits properties of an ideal multiferroic material, partially because of the high spin ($S=5/2$) and strong magnetic super-exchange interactions. We report the full range of spin dynamics in a bulk single crystal of (Lu$_{0.6}$Sc$_{0.4}$)FeO$_3$ (Sc doping to stabilize the hexagonal structure) measured via time-of-flight inelastic neutron scattering. Modeling with linear spin wave theory yields a nearest neighbor exchange coupling of $J$ = 4.0(2) meV (DFT calculations for $h$-LuFeO$_3$ predicted a value of 6.31 meV) and anisotropy values of $K_D$ = 0.17(1) meV (easy plane) and $K_A$~=~-0.05(1)~meV (local easy axis). It is observed that the magnon bandwidth of the spin wave spectra is twice as large for $h$-(Lu,Sc)FeO$_3$ as it is for $h$-LuMnO$_3$.

cond-mat.str-el↗

arXiv2018

Magnetic excitations of the Cu$^{2+}$ quantum spin chain in Sr$_3$CuPtO$_6$

We report the magnetic excitation spectrum as measured by inelastic neutron scattering for a polycrystalline sample of Sr$_3$CuPtO$_6$. Modeling the data by the 2+4 spinon contributions to the dynamical susceptibility within the chains, and with interchain coupling treated in the random phase approximation, accounts for the major features of the powder-averaged structure factor. The magnetic excitations broaden considerably as temperature is raised, persisting up to above 100 K and displaying a broad transition as previously seen in the susceptibility data. No spin gap is observed in the dispersive spin excitations at low momentum transfer, which is consistent with the gapless spinon continuum expected from the coordinate Bethe ansatz. However, the temperature dependence of the excitation spectrum gives evidence of some very weak interchain coupling.

cond-mat.str-el↗

arXiv2018

Soft tilt and rotational modes in the hybrid improper ferroelectric Ca$_{3}$Mn$_{2}$O$_{7}$

Raman spectroscopy is employed to probe directly the soft rotation and tilting modes, which are two primary order parameters predicted in the hybrid improper ferroelectric material Ca$_3$Mn$_2$O$_7$. We observe a giant softening of the 107-cm$^{-1}$ octahedron tilting mode by 26~cm$^{-1}$, on heating through the structural transition from a ferroelectric to paraelectric orthorhombic phase. This is contrasted by a small softening of the 150-cm$^{-1}$ rotational mode by 6~cm$^{-1}$. In the intermediate phase, the competing soft modes with different symmetries coexist, bringing about many-faceted anomalies in spin excitations and lattice vibrations. Our work demonstrates that the soft rotation and tilt patterns, relying on a phase-transition path, are a key factor in determining ferroelectric, magnetic, and lattice properties of Ca$_3$Mn$_2$O$_7$.

cond-mat.str-el↗

arXiv2018

Soft antiphase tilt of oxygen octahedra in the hybrid improper multiferroic Ca3Mn1.9Ti0.1O7

We report a single crystal neutron and x-ray diffraction study of the hybrid improper multiferroic Ca3Mn1.9Ti0.1O7 (CMTO), a prototypical system where the electric polarization arises from the condensation of two lattice distortion modes.With increasing temperature (T ), the out-of-plane, antiphase tilt of MnO6 decreases in amplitude while the in-plane, in-phase rotation remains robust and experiences abrupt changes across the first-order structural transition. Application of hydrostatic pressure (P) to CMTO at room temperature shows a similar effect. The consistent behavior under both T and P reveals the softness of antiphase tilt and highlights the role of the partially occupied d orbital of the transition-metal ions in determining the stability of the octahedral distortion. Polarized neutron analysis indicates the symmetry-allowed canted ferromagnetic moment is less than the 0.04 μB/Mn site, despite a substantial out-of-plane tilt of the MnO6 octahedra.

cond-mat.str-el↗

arXiv2017

Orphan spins and bound in-gap states in the $S={5\over2}$ antiferromagnet CaFe$_{2}$O$_{4}$

CaFe$_{2}$O$_{4}$ is an anisotropic $S={5\over 2}$ antiferromagnet with two competing $A$ ($\uparrow \uparrow \downarrow \downarrow$) and $B$ ($\uparrow \downarrow \uparrow \downarrow$) magnetic order parameters separated by static antiphase boundaries at low temperatures. Neutron diffraction and bulk susceptibility measurements, show that the spins near these boundaries are weakly correlated and a carry an uncompensated ferromagnetic moment that can be tuned with a magnetic field. Spectroscopic measurements find these spins are bound with excitation energies less than the bulk magnetic spin-waves and resemble the spectra from isolated spin-clusters. Localized bound orphaned spins separate the two competing magnetic order parameters in CaFe$_{2}$O$_{4}$.

cond-mat.mtrl-sci↗

arXiv2017

Hidden Antipolar Order Parameter and Entangled Neel-Type Charged Domain Walls in Hybrid Improper Ferroelectrics

Hybrid improper ferroelectricity (HIF) denotes a new class of polar instability by the mixture of two octahedral-distortion modes and can feature the coexistence of abundant head-to-head and tail-to-tail polar domains, of which the domain walls tend to be charged due to the respective screening charges with an opposite sign. However, no such coexisting carriers are available in the materials. Using group-theoretical, microscopic, and spectroscopic analyses, we established the existence of hidden antipolar order parameter in model HIF (Ca,Sr)3Ti2O7 by the condensation of a weak, previously unnoticed antipolar lattice instability, turning the order-parameter spaces to be multicomponent with the distinct polar-antipolar intertwining and accompanied formation of Neel-type twin-like antipolar domain walls (few nm) between the head-to-head and tail-to-tail domains. The finite-width Neel walls and correlated domain topology inherently lift the polar divergences between the domains, casting an emergent exemplification of charged domain-wall screening by an antipolar ingredient. Comparisons to topological defects in improper-ferroelectrics hexagonal manganites were discussed.

cond-mat.str-el↗

arXiv2017

Chiral Spin Mode on the Surface of a Topological Insulator

Using polarization-resolved resonant Raman spectroscopy, we explore collective spin excitations of the chiral surface states in a three dimensional topological insulator, Bi$_2$Se$_3$. We observe a sharp peak at 150 meV in the pseudovector $A_2$ symmetry channel of the Raman spectra. By comparing the data with calculations, we identify this peak as the transverse collective spin mode of surface Dirac fermions. This mode, unlike a Dirac plasmon or a surface plasmon in the charge sector of excitations, is analogous to a spin wave in a partially polarized Fermi liquid, with spin-orbit coupling playing the role of an effective magnetic field.

cond-mat.mtrl-sci↗