arXiv subjects

Choong H. Kim

Publications and source records attributed to Choong H. Kim.

At least 19 recordsLinked to original sources

arXiv2026

Strain-driven spin-flop transition and collapse of the giant magnon gap in the bilayer iridate Sr$_3$Ir$_2$O$_7$

The bilayer iridate Sr$_3$Ir$_2$O$_7$ is a $c$-axis collinear antiferromagnet, held there by a giant interlayer pseudodipolar anisotropy, whereas single-layer Sr$_2$IrO$_4$ cants in the $ab$ plane. We show from first principles that biaxial compression of a few percent ($\varepsilon_c\approx-2.4\%$) flops the easy axis of Sr$_3$Ir$_2$O$_7$ into the plane. A magnetic model Hamiltonian built from Wannier functions with no fitted parameter---reproducing the giant magnon gap of the bulk, so far known only from fits to experiment---identifies the mechanism. Compression collapses the interlayer exchange channel, whose straight Ir--O--Ir path weakens as the bent in-plane path strengthens. Hund's exchange sets the scale of the anisotropy and, beyond $J/U\approx0.15$, removes the collinear state altogether. The flop is not a rigid rotation---the ordered moments of the two states cross at $\varepsilon_c$---and it carries a stark fingerprint, in that the giant easy-axis magnon gap collapses to a gapless, Goldstone-like spectrum. Compressively strained films thus sit on a metamagnetic phase boundary ending in a zero-temperature bicritical point, a charge-neutral handle on spin--orbit-entangled order.

cond-mat.str-el↗

arXiv2023

Classification of magnetic order from electronic structure by using machine learning

Identifying the magnetic state of materials is of great interest in a wide range of applications, but direct identification is not always straightforward due to limitations in neutron scattering experiments. In this work, we present a machine-learning approach using decision-tree algorithms to identify magnetism from the spin-integrated excitation spectrum, such as the density of states. The dataset was generated by Hartree-Fock mean-field calculations of candidate antiferromagnetic orders on a Wannier Hamiltonian, extracted from first-principle calculations targeting BaOsO$_3$. Our machine learning model was trained using various types of spectral data, including local density of states, momentum-resolved density of states at high-symmetry points, and the lowest excitation energies from the Fermi level. Although the density of states shows good performance for machine learning, the broadening method had a significant impact on the model's performance. We improved the model's performance by designing the excitation energy as a feature for machine learning, resulting in excellent classification of antiferromagnetic order, even for test samples generated by different methods from the training samples used for machine learning.

cond-mat.mtrl-sci↗

arXiv2022

Ferroelectricity-driven phonon Berry curvature and non-linear phonon Hall transports

Berry curvature (BC) governs topological phases of matter and generates anomalous transport. When a magnetic field is applied, phonons can acquire BC indirectly through spin-lattice coupling, leading to a linear phonon Hall effect. Here, we show that polar lattice distortion directly couples to a phonon BC dipole, which causes a switchable non-linear phonon Hall effect. In a SnS monolayer, the in-plane ferroelectricity induces a phonon BC and leads to the phononic version of the non-volatile BC memory effect. As a new type of ferroelectricity-phonon coupling, the phonon Rashba effect emerges and opens a mass-gap in tilted Weyl phonon modes, resulting in a large phonon BC dipole. Furthermore, our ab initio non-equilibrium molecular dynamics simulations reveal that non-linear phonon Hall transport occurs in a controllable manner via ferroelectric switching. The ferroelectricity-driven phonon BC and corresponding non-linear phonon transports provide a novel scheme for constructing topological phononic transport/memory devices.

cond-mat.mes-hall↗

arXiv2022

Tuning orbital-selective phase transitions in a two-dimensional Hund's correlated system

Hund's rule coupling ($\textit{J}$) has attracted much attention recently for its role in the description of the novel quantum phases of multi orbital materials. Depending on the orbital occupancy, $\textit{J}$ can lead to various intriguing phases. However, experimental confirmation of the orbital occupancy dependency has been difficult as controlling the orbital degrees of freedom normally accompanies chemical inhomogeneities. Here, we demonstrate a method to investigate the role of orbital occupancy in $\textit{J}$ related phenomena without inducing inhomogeneities. By growing SrRuO$_3$ monolayers on various substrates with symmetry-preserving interlayers, we gradually tune the crystal field splitting and thus the orbital degeneracy of the Ru $\textit{t$_2$$_g$}$ orbitals. It effectively varies the orbital occupancies of two-dimensional (2D) ruthenates. Via in-situ angle-resolved photoemission spectroscopy, we observe a progressive metal-insulator transition (MIT). It is found that the MIT occurs with orbital differentiation: concurrent opening of a band insulating gap in the $\textit{d$_x$$_y$}$ band and a Mott gap in the $\textit{d$_x$$_z$$_/$$_y$$_z$}$ bands. Our study provides an effective experimental method for investigation of orbital-selective phenomena in multi-orbital materials.

cond-mat.str-el↗

arXiv2022

Heteroepitaxial control of Fermi liquid, Hund metal, and Mott insulator phases in the single-atomic-layer limit

Interfaces between dissimilar correlated oxides can offer devices with versatile functionalities. In that respect, manipulating and measuring novel physical properties of oxide heterointerfaces are highly desired. Yet, despite extensive studies, obtaining direct information on their momentum-resolved electronic structure remains a great challenge. This is because most correlated interfacial phenomena appear within a few atomic layers from the interface, thus limiting the application of available experimental probes. Here, we utilize atomic-scale epitaxy and photoemission spectroscopy to demonstrate the interface control of correlated electronic phases in atomic-scale ruthenate--titanate heterostructures. While bulk SrRuO$_3$ is a ferromagnetic metal, the heterointerfaces exclusively realize three distinct correlated phases in the single-atomic-layer limit. Our theory reveals that atomic-scale structural proximity effects lead to the emergence of Fermi liquid, Hund metal, and Mott insulator phases in the quantum-confined SrRuO$_3$. These results highlight the extensive interfacial tunability of electronic phases, hitherto hidden in the atomically thin correlated heterostructure.

cond-mat.str-el↗

arXiv2021

Observation of metallic electronic structure in a single-atomic-layer oxide

Correlated electrons in transition metal oxides (TMOs) exhibit a variety of emergent phases. When TMOs are confined to a single-atomic-layer thickness, experiments so far have shown that they usually lose diverse properties and become insulators. In an attempt to extend the range of electronic phases of the single-atomic-layer oxide, we search for a metallic phase in a monolayer-thick epitaxial SrRuO$_3$ film. Combining atomic-scale epitaxy and angle-resolved photoemission measurements, we show that the monolayer SrRuO$_3$ is a strongly correlated metal. Systematic investigation reveals that the interplay between dimensionality and electronic correlation makes the monolayer SrRuO$_3$ an incoherent metal with orbital-selective correlation. Furthermore, the unique electronic phase of the monolayer SrRuO$_3$ is found to be highly tunable, as charge modulation demonstrates an incoherent-to-coherent crossover of the two-dimensional metal. Our work emphasizes the potentially rich phases of single-atomic-layer oxides and provides a guide to the manipulation of their two-dimensional correlated electron systems.

cond-mat.str-el↗

arXiv2021

Hund's metallicity enhanced by van Hove singularity in cubic perovskite systems

A van Hove singularity (VHS) often significantly amplifies the electronic instability of a crystalline solid, including correlation-induced phenomena such as Hund's metallicity. We perform a systematic study on the interplay between Hund's coupling and electronic structures with a VHS focusing on Hund's metallicity. We construct a simplified tight-binding model targeting cubic perovskite materials and test the effects of the VHS utilizing dynamical mean-field theory with an exact diagonalization solver. The quasiparticle weight and the low-frequency power exponent of the self-energy provide a quantitative estimation of metallicity over the phase diagram. We find the VHS to substantially enhance Hund's metallicity. The results here suggest a range of parameters through which a VHS can bring great synergy with Hund's coupling.

cond-mat.str-el↗

arXiv2021

Observation of Kondo hybridization with an orbital-selective Mott phase in 4d Ca2-xSrxRuO4

The heavy fermion state with Kondo-hybridization (KH), usually manifested in f-electron systems with lanthanide or actinide elements, was recently discovered in several 3d transition metal compounds without f-electrons. However, KH has not yet been observed in 4d/5d transition metal compounds, since more extended 4d/5d orbitals do not usually form flat bands that supply localized electrons appropriate for Kondo pairing. Here, we report a doping- and temperature-dependent angle-resolved photoemission study on 4d Ca2-xSrxRuO4, which shows the signature of KH. We observed a spectral weight transfer in the γ-band, reminiscent of an orbital-selective Mott phase (OSMP). The Mott localized γ-band induces KH with the itinerant \b{eta}-band, resulting in spectral weight suppression around the Fermi level. Our work is the first to demonstrate the evolution of the OSMP with possible KH among 4d electrons, and thereby expands the material boundary of Kondo physics to 4d multi-orbital systems.

cond-mat.str-el↗

arXiv2021

Pressure-induced transition from Jeff=1/2 to S=1/2 states in CuAl2O4

The spin-orbit entangled (SOE) Jeff-state has been a fertile ground to study novel quantum phenomena. Contrary to the conventional weakly correlated Jeff=1/2 state of 4d and 5d transition metal compounds, the ground state of CuAl2O4 hosts a Jeff=1/2 state with a strong correlation of Coulomb U. Here, we report that surprisingly Cu2+ ions of CuAl2O4 overcome the otherwise usually strong Jahn-Teller distortion and instead stabilize the SOE state, although the cuprate has relatively small spin-orbit coupling. From the x-ray absorption spectroscopy and high-pressure x-ray diffraction studies, we obtained definite evidence of the Jeff=1/2 state with a cubic lattice at ambient pressure. We also found the pressure-induced structural transition to a compressed tetragonal lattice consisting of the spin-only S=1/2 state for pressure higher than Pc=8 GPa. This phase transition from the Mott insulating Jeff=1/2 to the S=1/2 states is a unique phenomenon and has not been reported before. Our study offers a rare example of the SOE Jeff-state under strong electron correlation and its pressure-induced transition to the S=1/2 state.

cond-mat.str-el↗

arXiv2020

Electric field driven octahedral rotation in perovskite

Rotation of MO6 (M = transition metal) octahedra is a key determinant of the physical properties of perovskite materials. Therefore, tuning physical properties, one of the most important goals in condensed matter research, may be accomplished by controlling octahedral rotation (OR). In this study, it is demonstrated that OR can be driven by an electric field in Sr$_2$RuO$_4$. Rotated octahedra in the surface layer of Sr$_2$RuO$_4$ are restored to the unrotated bulk structure upon dosing the surface with K. Theoretical investigation shows that OR in Sr$_2$RuO$_4$ originates from the surface electric field, which can be tuned via the screening effect of the overlaid K layer. This work establishes not only that variation in the OR angle can be induced by an electric field, but also provides a way to control OR, which is an important step towards in situ control of the physical properties of perovskite oxides.

cond-mat.mtrl-sci↗

arXiv2020

Interplay between spin-orbit coupling and van Hove singularity in the Hund's metallicity of Sr$_2$RuO$_4$

We investigate the dynamical properties of Sr$_2$RuO$_4$ at zero and very low temperature using density functional theory plus dynamical mean-field theory with an exact diagonalization solver. By considering rotationally invariant local interaction, we examine how Hund's coupling and spin-orbit coupling affect the correlated nature of the system. In the absence of Hund's coupling, the system shows a Fermi liquid behavior over the entire range of temperatures we consider. We confirm that the Fermi liquid persists at zero temperature even with nonzero Hund's coupling; however, at sufficient temperatures Hund's coupling significantly reduces the Fermi liquid regime and the system evolves into a typical Hund's metal. At the bare electronic occupancy of Sr$_2$RuO$_4$ ($t_{2g}^4$), a stronger Hund's metallicity accompanies a larger long-time correlator. Remarkably, electron doping further destabilizes the Fermi liquid even though the long-time correlator and magnetic fluctuations decrease upon doping. This suppression of the Fermi liquid is driven by the van Hove singularity above the Fermi level in Sr$_2$RuO$_4$, combined with an enhanced Van Vleck susceptibility by spin-orbit coupling. Such findings point to the important role that electronic structure plays in the behavior of Hund's metals, in addition to magnetic fluctuations.

cond-mat.str-el↗

arXiv2020

Spin-orbit coupling effects on spin-phonon coupling in Cd2Os2O7

Spin-orbit coupling (SOC) is essential in understanding the properties of 5d transition metal compounds, whose SOC value is large and almost comparable to other key parameters. Over the past few years, there have been numerous studies on the SOC-driven effects of the electronic bands, magnetism, and spin-orbit entanglement for those materials with a large SOC. However, it is less studied and remains an unsolved problem in how the SOC affects the lattice dynamics. We, therefore, measured the phonon spectra of 5d pyrochlore Cd2Os2O7 over the full Brillouin zone to address the question by using inelastic x-ray scattering (IXS). Our main finding is a visible mode-dependence in the phonon spectra, measured across the metal-insulator transition at 227 K. We examined the SOC strength dependence of the lattice dynamics and its spin-phonon (SP) coupling, with first-principle calculations. Our experimental data taken at 100 K are in good agreement with the theoretical results obtained with the optimized U = 2.0 eV with SOC. By scaling the SOC strength and the U value in the DFT calculations, we demonstrate that SOC is more relevant than U to explaining the observed mode-dependent phonon energy shifts with temperature. Furthermore, the temperature dependence of the phonon energy can be effectively described by scaling SOC. Our work provides clear evidence of SOC producing a non-negligible and essential effect on the lattice dynamics of Cd2Os2O7 and its SP coupling.

cond-mat.mtrl-sci↗

arXiv2019

Ultrafast dynamics in the Lifshitz-type 5${d}$ pyrochlore antiferromagnet Cd$_{2}$Os$_{2}$O$_{7}$

We investigate the ultrafast dynamics of Cd$_2$Os$_2$O$_7$, a prototype material showing a Lifshitz-type transition as a function of temperature. In the paramagnetic metallic state, the photo-reflectivity shows a sub-picosecond relaxation, followed by a featureless small offset. In the antiferromagnetic state slightly below $T_N$, however, the photo-reflectivity resurges over hundreds of picoseconds, which goes beyond the usual realm of the effective-temperature model. Our observations are consistent with the Lifshitz phase transition of Cd$_2$Os$_2$O$_7$ driven by the evolution of the local magnetic moment.

cond-mat.str-el↗

arXiv2019

Theoretical evidence of spin-orbital-entangled $J_{\mathbf{eff}}$=1/2 state in the 3$d$ transition metal oxide CuAl$_2$O$_4$

Transition metal oxides exhibit various competing phases and exotic phenomena depending on how their reaction to the rich degeneracy of the $d$-orbital. Large spin-orbit coupling (SOC) reduces this degeneracy in a unique way by providing a spin-orbital-entangled ground state for 4$d$ and 5$d$ transition metal compounds. In particular, the spin-orbital-entangled Kramers doublet, known as the $J_{\mathbf{eff}}$=1/2 pseudospin, appears in layered iridates and $α$-RuCl$_3$, manifesting a relativistic Mott insulating phase. Such entanglement, however, seems barely attainable in 3$d$ transition metal oxides, where the SOC is small and the orbital angular momentum is easily quenched. From experimental and theoretical evidence, here we report on the CuAl$_2$O$_4$ spinel as the first example of a $J_{\mathbf{eff}}$=1/2 Mott insulator in 3$d$ transition metal compounds. Based on the experimental study, including synthesis of the cubic CuAl$_2$O$_4$ single crystal, density functional theory and dynamical mean field theory calculations reveal that the $J_{\mathbf{eff}}$=1/2 state survives the competition with an orbital-momentum-quenched $S$=1/2 state. The electron-addition spectra probing unoccupied states are well described by the $j_{\mathbf{eff}}$=1/2 hole state, whereas electron-removal spectra have a rich multiplet structure. The fully relativistic entity found in CuAl$_2$O$_4$ provides new insight into the untapped regime where the spin-orbital-entangled Kramers pair coexists with strong electron correlation.

cond-mat.str-el↗

arXiv2019

Evidence of structural evolution in Sr2RhO4 studied by time-resolved optical reflectivity spectroscopy

We investigate ultrafast dynamics from photoinduced reflectivity of Sr2RhO4 by using femtosecond near-infrared pulses. We observe a clear temperature-dependent anomaly in its electronic dynamics which slows down below 160 K. In addition, coherent oscillations of the A1g symmetric 5.3-THz phonon exhibit a 90-degree shift in its initial phase across TS, indicating a structural change in octahedral rotation distortions. We propose that octahedral structure in Sr2RhO4 evolves at around TS, and it can influence on the non-equilibrium dynamics of photoinduced carriers as well as real-time phonon responses.

cond-mat.str-el↗

arXiv2019

Two-dimensional Peierls instability via zone boundary Dirac line nodes in layered perovskite oxides

Interplay of Fermi surface topology and electron correlation is the quintessential ingredient underlying spontaneous symmetry breaking in itinerant electronic systems. In one-dimensional (1D) systems at half-filling, the inherent Fermi surface nesting makes the translationally invariant metallic state unstable, which is known as Peierls instability. Extending the scope of Peierls instability to two (2D) or three dimensions (3D), however, is not straightforward, since the Fermi surface in higher dimensions is generally not nested. In this work, we show that a perfectly nested Fermi surface can be realized in a class of 2D perovskite oxides, giving rise to 2D Peierls instability. Here the central role is played by the zone boundary Dirac line node (DLN) protected by two orthogonal glide mirrors induced by the rotation of oxygen octahedra. Especially, at a critical angle of the octahedron rotation, the zone-boundary DLN flattens, leading to logarithmically diverging susceptibility. We propose the 2D Peierls instability driven by dispersionless DLN as a principle mechanism for spontaneous symmetry breaking in various layered perovskite oxides including the antiferromagnetism of Sr$_2$IrO$_4$. As a clear signature of the 2D Peierls instability, we predict that the magnetic domain wall in Sr$_2$IrO$_4$ hosts localized soliton modes.

cond-mat.str-el↗

arXiv2019

Crystalline topological Dirac semimetal phase in rutile structure $β'$-PtO$_2$

Based on first-principles calculations and symmetry analysis, we propose that a transition metal rutile oxide, in particular $β'$-PtO$_2$, can host a three-dimensional topological Dirac semimetal phase. We find that $β'$-PtO$_2$ possesses a linked nodal rings structure when spin-orbit coupling is neglected. Incorporating spin-orbit coupling gaps the nodal rings, while preserving a single pair of three-dimensional Dirac points protected by a screw rotation symmetry. This Dirac point is created by a band inversion of two $d$ bands, which is a realization of a DSM phase in correlated electron systems. Moreover, a mirror plane in the momentum space carries a nontrivial mirror Chern number $n_M = -2$, which distinguishes $β'$-PtO$_2$ from the Dirac semimetals known so far, such as Na$_3$Bi and Cd$_3$As$_2$. If we apply a perturbation that breaks the rotation symmetry and preserves the mirror symmetry, the Dirac points are gapped and the system becomes a topological crystalline insulator.

cond-mat.str-el↗

arXiv2018

Orbital-selective confinement effect of Ru $4d$ orbitals in SrRuO$_3$ ultrathin film

The electronic structure of SrRuO$_3$ thin film with thickness from 50 to 1 unit cell (u.c.) is investigated via the resonant inelastic x-ray scattering (RIXS) technique at the O K-edge to unravel the intriguing interplay of orbital and charge degrees of freedom. We found that orbital-selective quantum confinement effect (QCE) induces the splitting of Ru $4d$ orbitals. At the same time, we observed a clear suppression of the electron-hole continuum across the metal-to-insulator transition (MIT) occurring at the 4 u.c. sample. From these two clear observations we conclude that QCE gives rise to a Mott insulating phase in ultrathin SrRuO$_3$ films. Our interpretation of the RIXS spectra is supported by the configuration interaction calculations of RuO$_6$ clusters.

cond-mat.str-el↗