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Beom Hyun Kim

Publications and source records attributed to Beom Hyun Kim.

At least 19 recordsLinked to original sources

Unconventional and Fragile Magnetic Exciton in a van der Waals Quantum Magnet

The recently discovered magnetic exciton in the van der Waals (vdW) antiferromagnet NiPS3 exemplifies these phenomena, exhibiting several distinctive characteristics. Despite extensive investigation, much of its physics remains unresolved, with key questions about why the NiPS3 magnetic exciton is so sharp and optically bright despite the nominally spin-forbidden transition, posing significant challenges to a proper understanding and practical manipulation of the exciton. An urgent question is to what extent it is due to chemical disorder, magnetic weakening, lattice modification, or intrinsic instability of the bright exciton itself: answers to which will put stringent constraints on possible theoretical models. Here we address these questions using hydrostatic pressure as a clean, continuous, reversible, and in-situ tuning parameter. We find that the sharp photoluminescence peak is drastically suppressed by as little as 0.4 GPa and completely quenched by 1.5 GPa, with demonstrating its reversibility. Crucially, this bright-to-dark conversion occurs without magnetic, crystallographic, or electronic reconstruction despite an increase in the Neel temperature, as established by Raman, X-ray absorption, nuclear magnetic resonance spectroscopy, and first-principles many-body calculations. Our results demonstrate that the optical brightness of the magnetic exciton is independent of chemical disorder, lattice expansion, and weakening of magnetic order, indicating that a higher-order correlated mechanism governs the bright exciton. We further propose experimentally constrained microscopic scenarios involving exciton pairing, crystal-field-controlled spin-orbit mixing, and symmetry breaking, providing a framework for future tests of entangled magnetic exciton in correlated quantum magnets.

cond-mat.mtrl-sci

X-ray magnetic circular dichroism and resonant inelastic X-ray scattering explained: role of many-body correlation and valence fluctuations

X-ray magnetic circular dichroism (XMCD) and resonant inelastic X-ray scattering with magnetic circular dichroism (RIXS-MCD) provide unparalleled insights into the electronic and magnetic dynamics of complex materials. However, interpreting their spectra in mixed-valence systems remains challenging due to intricate many-body interactions and enhanced charge fluctuations. In this study, by utilizing the Anderson impurity model with a full consideration of charge transfer (CT), many-body core-valence exchange correlation (CVEC) effects, and Jahn-Teller (JT) distortions, we systematically investigate the XMCD and RIXS-MCD spectra for a prototypical mixed-valence ferromagnet, La$_{0.7}$Sr$_{0.3}$MnO$_3$ film. We demonstrate that simple calculation with limited CT effects fails to capture characteristic substructures observed experimentally. In contrast, an adequate treatment of CT and CVEC effects yields a more consistent description of both XMCD and RIXS-MCD spectra, providing practical guidance for the interpretation of dichroic x-ray spectroscopies in mixed-valence transition-metal oxides. Furthermore, we discuss the role of the JT effect in Mn$^{3+}$ ions in the determination of their spectra.

cond-mat.str-el

Microscopic evidence for a Zhang-Rice triplet state in the van der Waals antiferromagnet, NiPS$_3$

Quantum-entangled states underpin many emergent phenomena in quantum materials, yet their direct experimental identification remains a challenge. NiPS$_3$, a van der Waals antiferromagnet exhibiting a resolution-limited magnetic exciton in its ordered phase, has been proposed to host a many-body entangled Zhang-Rice triplet state. Here, using $^{33}$S nuclear magnetic resonance (NMR) on $^{33}$S-enriched NiPS$_3$ single crystals, we provide microscopic evidence for this charge-transfer state. The $^{33}$S and $^{31}$P Knight shifts as a function of temperature reveal a unified spin-triplet configuration arising from strong hybridization between a self-doped hole in the S $3p$ orbitals and a hole in Ni $3d$ orbitals. Furthermore, the $^{33}$S nuclear spin-lattice relaxation rate exhibits a power-law divergence as it approaches the Néel temperature $T_N=155$ K, indicating critical slowing down of collective charge fluctuations consistent with spin-nematic correlations. These results reveal a spin-charge-intertwined ground state and establish the microscopic foundation for the exceptional coherence of the magnetic exciton in NiPS$_3$.

cond-mat.str-el

Direction-selective intertwined charge, orbital, and lattice orders under uniaxial strain in hole-doped manganite: La0.75Ca0.25MnO3

The complex interplay of charge, spin, orbital, and lattice degrees of freedom governs emergent phases in quantum materials, making strain a powerful control parameter. Recent advances in free-standing layer techniques have enabled extreme strains of nearly 8%, opening access to novel and often unexpected electronic and magnetic phases. Here, using a density functional theory approach, we investigate the effect of direction-selective uniaxial strain on the prototypical Jahn-Teller system La1-xCaxMnO3 (x = 0.25). We find that different strain directions stabilize qualitatively distinct structural, charge, and orbital responses, rather than merely different strengths of the same phase. In particular, extreme uniaxial strain selectively induces cooperative Jahn-Teller, breathing-like, and site-selective modulations, thereby enabling previously inaccessible intertwined orders in manganites. These results establish direction-selective uniaxial strain as a powerful and selective route for engineering emergent phases in quantum materials.

cond-mat.str-el

Intertwined Orders in a Quantum-Entangled Metal

Entanglement underpins quantum information processing and computing, yet its experimental quantification in complex, many-body condensed matter systems remains a considerable challenge. Here, we reveal a highly entangled electronic phase proximate to a quantum metal-insulator transition, identified by resonant inelastic x-ray scattering interferometry. This approach reveals that entanglement across atomic sites generates characteristic interference patterns, which our model accurately reproduces, enabling extraction of a full entanglement spectrum and resolution of the underlying quantum states. Our analysis of the pyrochlore iridate Nd2Ir2O7 demonstrates that the system undergoes pronounced quantum fluctuations in its spin, orbital and charge degrees of freedom, even in the presence of a long-range 'all-in-all-out' antiferromagnetic order. Importantly, the observed entanglement signatures facilitate the coexistence of multiple exotic symmetry-breaking orders. Complementary investigations using Raman spectroscopy corroborate the presence of these hidden orders and their emergent excitations. In particular, we observe a two-magnon-bound state below the lowest single-magnon excitation energy, which, together with split phonon modes, provides strong evidence for cubic symmetry-breaking orders of magnetic origin juxtaposed with the all-in-all-out order. Our work thus establishes a direct link between quantum entanglement and emergent unconventional orders, opening new avenues for investigating quantum materials.

cond-mat.str-el

Magnetoelectric effect in van der Waals magnets

The magnetoelectric (ME) effect is a fundamental concept in modern condensed matter physics and represents the electrical control of magnetic polarisations or vice versa. Two-dimensional (2D) van-der-Waals (vdW) magnets have emerged as a new class of materials and exhibit novel ME effects with diverse manifestations. This review emphasizes some important recent discoveries unique to vdW magnets: multiferroicity on two dimensions, spin-charge correlation, atomic ME effect and current-induced intrinsic spin-orbit torque, and electrical gating control and magnetic control of their electronic properties. We also highlight the promising route of utilizing quantum magnetic hetero- or homo-structures to engineer the ME effect and corresponding spintronic and optoelectronic device applications. Due to the intrinsic two-dimensionality, vdW magnets with those ME effects are expected to form a new, exciting research direction.

cond-mat.mtrl-sci

Highly Tunable Ru-dimer Molecular Orbital State in 6H-perovskite Ba$_3$MRu$_2$O$_9$

Molecular orbital (MO) systems with clusters of heavy transition metal (TM) ions are one of the most important classes of model materials for studying the interplay between local physics and effects of itinerancy. Despite a large number of candidates identified in the family of 4d TM materials, an understanding of their physics from competing \textit{microscopic} energy scales is still missing. We bridge this gap by reporting the first resonant inelastic X-ray scattering (RIXS) measurement on a well-known series of Ru dimer systems with a 6H-perovskite structure, Ba$_3$MRu$_2$O$_9$ (M$^{3+}$=In$^{3+}$, Y$^{3+}$, La$^{3+}$). Our RIXS measurements reveal an extremely fragile MO state in these Ru dimer compounds, evidenced by an abrupt change in the RIXS spectrum accompanying a tiny change in the local structure tuned by the M-site ion. By modelling the RIXS spectra, we attribute the enhanced electronic instability in Ba$_3$MRu$_2$O$_9$ to the combined effect of a large hopping and a small spin-orbit coupling in the Ru dimers. The unique combination of energy scales uncovered in the present study make Ru MO systems ideal model systems for studying quantum phase transitions with molecular orbitals.

cond-mat.str-el

Eigenstate switching of topologically ordered states using non-Hermitian perturbations

Topologically ordered phases have robust degenerate ground states against the local perturbations, providing a promising platform for fault-tolerant quantum computation. Despite of the non-local feature of the topological order, we find that local non-Hermitian perturbations can induce the transition between the topologically ordered ground states. In this work, we study the toric code in the presence of non-Hermitian perturbations. By controlling the non-Hermiticity, we show that non-orthogonal ground states can exhibit an eigenstate coalescence and have the spectral singularity, known as an exceptional point (EP). We explore the potential of the EPs in the control of topological order. Adiabatic encircling EPs allows for the controlled switching of eigenstates, enabling dynamic manipulation between the ground state degeneracy. Interestingly, we show a property of our scheme that arbitrary strengths of local perturbations can induce the EP and eigenstate switching. Finally, we also show the orientation-dependent behavior of non-adiabatic transitions (NAT) during the dynamic encirclement around an EP. Our work shows that control of the non-Hermiticity can serve as a promising strategy for fault-tolerant quantum information processing.

cond-mat.mes-hall

Non-local features of the spin-orbit exciton in Kitaev materials

A comparative resonant inelastic x-ray scattering (RIXS) study of three well-known Kitaev materials is presented: $α$-Li$_2$IrO$_3$, Na$_2$IrO$_3$, and $α$-RuCl$_3$. Despite similar low-energy physics, these materials show distinct electronic properties, such as the large difference in the size of the charge gap. The RIXS spectra of the spin-orbit exciton for these materials show remarkably similar three-peak features, including sharp low energy peak (peak A) as well as transitions between $j_{\text{eff}}=1/2$ and $j_{\text{eff}}=3/2$ states. Comparison of experimental spectra with cluster calculations reveals that the observed three-peak structure reflects the significant role that non-local physics plays in the electronic structure of these materials. In particular, the low-energy peak A arises from a holon-doublon pair rather than a conventional particle-hole exciton as proposed earlier. Our study suggests that while spin-orbit assisted Mott insulator is still the best description for these materials, electron itinerancy cannot be ignored when formulating low-energy Hamiltonian of these materials.

cond-mat.str-el

Collective non-Hermitian skin effect: Point-gap topology and the doublon-holon excitations in non-reciprocal many-body systems

Open quantum systems provide a plethora of exotic topological phases of matter that has no Hermitian counterpart. Non-Hermitian skin effect, macroscopic collapse of bulk states to the boundary, has been extensively studied in various experimental platforms. However, it remains an open question whether such topological phases persist in the presence of many-body interactions. Notably, previous studies have shown that the Pauli exclusion principle suppresses the skin effect. In this study, we present a compelling counterexample by demonstrating the presence of the skin effect in doublon-holon excitations. While the ground state of the spin-half Hatano-Nelson model shows no skin effect, the doublon-holon pairs, as its collective excitations, display the many-body skin effect even in strong coupling limit. We rigorously establish the robustness of this effect by revealing a bulk-boundary correspondence mediated by the point gap topology within the many-body energy spectrum. Our findings underscore the existence of non-Hermitian topological phases in collective excitations of many-body interacting systems.

cond-mat.str-el

Multiferroic-enabled magnetic exciton in 2D quantum entangled van der Waals antiferromagnet NiI2

Matter-light interaction is at the center of diverse research fields from quantum optics to condensed matter physics, opening new fields like laser physics. A magnetic exciton is one such rare example found in magnetic insulators. However, it is relatively rare to observe that external variables control matter-light interaction. Here, we report that the broken inversion symmetry of multiferroicity can act as an external knob enabling the magnetic exciton in van der Waals antiferromagnet NiI2. We further discover that this magnetic exciton arises from a transition between Zhang-Rice-triplet and Zhang-Rice-singlet's fundamentally quantum entangled states. This quantum entanglement produces an ultra-sharp optical exciton peak at 1.384 eV with a 5 meV linewidth. Our work demonstrates that NiI2 is two-dimensional magnetically ordered with an intrinsically quantum entangled ground state.

cond-mat.str-el

The field-angle anisotropy of proximate Kitaev systems under an in-plane magnetic field

We have investigated the field-angle behaviors of magnetic excitations under an in-plane magnetic field for proximate Kitaev systems. By employing the exact diagonalization method in conjunction with the linear spin wave theory, we have demonstrated that the magnetic excitation gap in the polarized phase is determined by the magnon excitation at $M$ points and has a strong anisotropy with respect to the field direction in the vicinity of the critical field limit. The specific heat from this magnon excitation bears qualitatively the same anisotropic behaviors as expected one for the non-Abelian spin liquid phase in the Kitaev model and experimentally observed one of the intermediate phases in $α$-RuCl$_3$.

cond-mat.str-el

Exciton-driven antiferromagnetic metal in a correlated van der Waals insulator

Collective excitations of bound electron-hole pairs -- known as excitons -- are ubiquitous in condensed matter, emerging in systems as diverse as band semiconductors, molecular crystals, and proteins. Recently, their existence in strongly correlated electron materials has attracted increasing interest due to the excitons' unique coupling to spin and orbital degrees of freedom. The non-equilibrium driving of such dressed quasiparticles offers a promising platform for realizing unconventional many-body phenomena and phases beyond thermodynamic equilibrium. Here, we achieve this in the van der Waals correlated insulator NiPS$_3$ by photoexciting its newly discovered spin-orbit-entangled excitons that arise from Zhang-Rice states. By monitoring the time evolution of the terahertz conductivity, we observe the coexistence of itinerant carriers produced by exciton dissociation and the long-wavelength antiferromagnetic magnon that coherently precesses in time. These results demonstrate the emergence of a transient metallic state that preserves long-range antiferromagnetism, a phase that cannot be reached by simply tuning the temperature. More broadly, our findings open an avenue toward the exciton-mediated optical manipulation of magnetism.

cond-mat.str-el

Modulating Curie Temperature and Magnetic Anisotropy in Nanoscale Layered Cr_{2}Te_{3} Films: Implications for Room-Temperature Spintronics

Nanoscale layered ferromagnets have demonstrated fascinating two-dimensional magnetism down to atomic layers, providing a peculiar playground of spin orders for investigating fundamental physics and spintronic applications. However, strategy for growing films with designed magnetic properties is not well established yet. Herein, we present a versatile method to control the Curie temperature (T_{C}) and magnetic anisotropy during growth of ultrathin Cr_{2}Te_{3} films. We demonstrate increase of the TC from 165 K to 310 K in sync with magnetic anisotropy switching from an out-of-plane orientation to an in-plane one, respectively, via controlling the Te source flux during film growth, leading to different c-lattice parameters while preserving the stoichiometries and thicknesses of the films. We attributed this modulation of magnetic anisotropy to the switching of the orbital magnetic moment, using X-ray magnetic circular dichroism analysis. We also inferred that different c-lattice constants might be responsible for the magnetic anisotropy change, supported by theoretical calculations. These findings emphasize the potential of ultrathin Cr_{2}Te_{3} films as candidates for developing room-temperature spintronics applications and similar growth strategies could be applicable to fabricate other nanoscale layered magnetic compounds.

cond-mat.mtrl-sci

Interplay between multipolar spin interactions, Jahn-Teller effect and electronic correlation in a $J_{eff}=\frac{3}{2}$ insulator

In this work we study the complex entanglement between spin interactions, electron correlation and Janh-Teller structural instabilities in the 5d$^1$ $J_{eff}=\frac{3}{2}$ spin-orbit coupled double perovskite $\rm Ba_2NaOsO_6$ using first principles approaches. By combining non-collinear magnetic calculations with multipolar pseudospin Hamiltonian analysis and many-body techniques we elucidate the origin of the observed quadrupolar canted antifferomagnetic. We show that the non-collinear magnetic order originates from Jahn-Teller distortions due to the cooperation of Heisenberg exchange, quadrupolar spin-spin terms and both dipolar and multipolar Dzyaloshinskii-Moriya interactions. We find a strong competition between ferromagnetic and antiferromagnetic canted and collinear quadrupolar magnetic phases: the transition from one magnetic order to another can be controlled by the strength of the electronic correlation ($U$) and by the degree of Jahn-Teller distortions.

cond-mat.str-el

Proximate Kitaev system for an intermediate magnetic phase in in-plane magnetic fields

Motivated by the magnetic phase transition of a proximate Kitaev system $α$-RuCl$_3$ in the presence of a magnetic field, we study the simplest but essential quantum spin model with the ferromagnetic nearest neighboring (NN) Kitaev interaction and additional antiferromagnetic third NN Heisenberg interaction. Employing both exact diagonalization and density matrix renormalization group methods, we demonstrate that the model shows the magnetic phase transition from the zigzag order phase to the spin polarized phase through an intermediate phase in both cases when an in-plane magnetic field is applied perpendicular to the NN bond direction and when an out-of-plane field is applied, in good agreement with experimental observations. Furthermore, we verify that additional symmetric off-diagonal $Γ$ interaction and ferromagnetic Heisenberg interaction between NN spins can both suppress the intermediate phase with the in-plane field. Our result gives important clues on determining relevant interactions in the field-induced magnetic phase transition of proximate Kiteav systems.

cond-mat.str-el

Topological property of a $t_{2g}^5$ system with a honeycomb lattice structure

A $t_{2g}^5$ system with a honeycomb lattice structure such as Na$_2$IrO$_3$ was firstly proposed as a topological insulator even though Na$_2$IrO$_3$ and its isostructural materials in nature have been turned out to be a Mott insulator with magnetic order. Here we theoretically revisit the topological property based on a minimal tight-binding Hamiltonian for three $t_{2g}$ bands incorporating a strong spin orbit coupling and two types of the first nearest neighbor (NN) hopping channel between transition metal ions, i.e., the hopping ($t_1$) mediated by edge-shared ligands and the direct hopping ($t_1'$) between $t_{2g}$ orbitals via $ddσ$ bonding. We demonstrate that the topological phase transition takes place by varying only these hopping parameters with the relative strength parametrized by $θ$, i.e., $t_1=t\cosθ$ and $t_1'=t\sinθ$. We also explore the effect of the second and third NN hopping channels, and the trigonal distortion on the topological phase for the whole range of $θ$. Furthermore, we examine the electronic and topological phases in the presence of on-site Coulomb repulsion $U$. Employing the cluster perturbation theory, we show that, with increasing $U$, a trivial or topological band insulator in the absence of $U$ can be transferred into a Mott insulator with nontrivial or trivial band topology. We also show that the main effect of the Hund's coupling can be understood simply as the renormalization of $U$. We briefly discuss the relevance of our results to the existing materials.

cond-mat.str-el

Spin-orbital excitons and their potential condensation in pentavalent iridates

We investigate magnetic excitations in iridium insulators with pentavalent Ir$^{5+}$ ($5d^4$) ions with strong spin-orbit coupling. We obtain a microscopic model based on the local Ir$^{5+}$ multiplets involving $J=0$ (singlet), $J=1$ (triplet), and $J=2$ (quintet) spin-orbital states. We get effective interactions between these multiplets on square and face-centered-cubic (fcc) structures of magnetic ions in the layered-perovskites and the double-perovkites, in particular Ba$_2$YIrO$_6$. Further, we derive an effective spin-orbital Hamiltonian in terms of bond bosons and explore possible instabilities towards magnetic and quadrupole orderings. Additionally, we study charge excitations with help of the variational cluster perturbation theory and calculate the electronic charge gap as a function of hopping and Coulomb interactions. Based on both electronic and magnetic phase diagrams, we verify the possibility of excitonic magnetism due to condensation of spin-orbital excitons in Ir$^{5+}$ iridates.

cond-mat.str-el