arXiv subjects

Hyeong-Do Kim

Publications and source records attributed to Hyeong-Do Kim.

At least 19 recordsLinked to original sources

arXiv2026

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↗

arXiv2024

Using magnetic dynamics to measure the spin gap in a candidate Kitaev material

Materials potentially hosting Kitaev spin-liquid states are considered crucial for realizing topological quantum computing. However, the intricate nature of spin interactions within these materials complicates the precise measurement of low-energy spin excitations indicative of fractionalized excitations. Using Na$_{2}$Co$_2$TeO$_{6}$ as an example, we study these low-energy spin excitations using the time-resolved resonant elastic x-ray scattering (tr-REXS). Our observations unveil remarkably slow spin dynamics at the magnetic peak, whose recovery timescale is several nanoseconds. This timescale aligns with the extrapolated spin gap of $\sim$ 1 $μ$eV, obtained by density matrix renormalization group (DMRG) simulations in the thermodynamic limit. The consistency demonstrates the efficacy of tr-REXS in discerning low-energy spin gaps inaccessible to conventional spectroscopic techniques.

cond-mat.str-el↗

arXiv2022

Kondo interaction in FeTe and its potential role in the magnetic order

Finding d-electron heavy fermion (HF) states has been an important topic as the diversity in d-electron materials can lead to many exotic Kondo effect-related phenomena or new states of matter such as correlation-driven topological Kondo insulator or cooperation between long-range magnetism and Kondo lattice behavior. Yet, obtaining direct spectroscopic evidence for a d-electron HF system has been elusive to date. Here, we report the observation of Kondo lattice behavior in an antiferromagnetic metal, FeTe, via angle-resolved photoemission spectroscopy (ARPES) and transport properties measurements. The Kondo lattice behavior is represented by the emergence of a sharp quasiparticle at low temperatures. The transport property measurements confirm the low-temperature Fermi liquid behavior and reveal successive coherent-incoherent crossover upon increasing temperature. We interpret the Kondo lattice behavior as a result of hybridization between localized Fe 3dxy and itinerant Te 5pz orbitals. Our interpretation is further evidenced by Fano-type tunneling spectra which accompany a hybridization gap. Our observations strongly suggest unusual cooperation between Kondo lattice behavior and long-range magnetic order.

cond-mat.str-el↗

arXiv2021

Optical excitation of electromagnons in hexaferrite

Understanding ultrafast magnetization dynamics on the microscopic level is of strong current interest due to the potential for applications in information storage. In recent years, the spin-lattice coupling has been recognized to be essential for ultrafast magnetization dynamics. Magnetoelectric multiferroics of type II possess intrinsic correlations among magnetic sublattices and electric polarization (P) through spin-lattice coupling, enabling fundamentally coupled dynamics between spins and lattice. Here we report on ultrafast magnetization dynamics in a room-temperature multiferroic hexaferrite possessing ferrimagnetic and antiferromagnetic sublattices, revealed by time-resolved resonant x-ray diffraction. A femtosecond above-bandgap excitation triggers a coherent magnon in which the two magnetic sublattices entangle and give rise to a transient modulation of P. A novel microscopic mechanism for triggering the coherent magnon in this ferrimagnetic insulator based on the spin-lattice coupling is proposed. Our finding opens up a novel but general pathway for ultrafast control of magnetism.

cond-mat.str-el↗

arXiv2021

4D visualization of the photoexcited coherent magnon by an X-ray free electron laser

X-ray free electron lasers (XFEL) create femtosecond X-ray pulses with high brightness and high longitudinal coherence allowing to extend X-ray spectroscopy and scattering techniques into the ultrafast time-domain. These X-rays are a powerful probe for studying coherent quasiparticle excitations in condensed matter triggered by an impulsive optical laser pump. However, unlike coherent phonons, other quasiparticles have been rarely observed due to small signal changes and lack of standards for the identification. Here, we exploit resonant magnetic X-ray diffraction using an XFEL to visualize a photoexcited coherent magnon in space and time. Large intensity oscillations in antiferromagnetic and ferromagnetic Bragg reflections from precessing moment are observed in a multiferroic Y-type hexaferrite. The precession trajectory reveals that a large, long-lived, photoinduced magnetic-field changes the net magnetization substantially through the large-amplitude of the magnon. This work demonstrates an efficient XFEL probe for the coherent magnon in the spotlight for opto-spintronics application.

cond-mat.str-el↗

arXiv2021

Ultrafast renormalization of the onsite Coulomb repulsion in a cuprate superconductor

Ultrafast lasers are an increasingly important tool to control and stabilize emergent phases in quantum materials. Among a variety of possible excitation protocols, a particularly intriguing route is the direct light-engineering of microscopic electronic parameters, such as the electron hopping and the local Coulomb repulsion (Hubbard $U$). In this work, we use time-resolved x-ray absorption spectroscopy to demonstrate the light-induced renormalization of the Hubbard $U$ in a cuprate superconductor, La$_{1.905}$Ba$_{0.095}$CuO$_4$. We show that intense femtosecond laser pulses induce a substantial redshift of the upper Hubbard band, while leaving the Zhang-Rice singlet energy unaffected. By comparing the experimental data to time-dependent spectra of single- and three-band Hubbard models, we assign this effect to a $\sim140$ meV reduction of the onsite Coulomb repulsion on the copper sites. Our demonstration of a dynamical Hubbard $U$ renormalization in a copper oxide paves the way to a novel strategy for the manipulation of superconductivity, magnetism, as well as to the realization of other long-range-ordered phases in light-driven quantum materials.

cond-mat.str-el↗

arXiv2021

Semimetallic Nature and Magnetic Polarons in EuB6 Studied by Angle-Resolved Photoemission Spectroscopy

Temperature-dependent angle-resolved photoemission spectroscopy (ARPES) was carried out on single-crystalline EuB6 samples. By measuring ARPES spectra in an extended Brillouin zone, a B 2p hole pocket centered at the X point is clearly observed, thus proving the semimetallic nature of EuB6. Below the Curie temperature TC, ARPES spectra show two B 2p bands of which separation is due to an exchange interaction between local Eu 4f and itinerant B 2p electrons. The exchange splitting becomes smaller as the temperature increases and disappears well above TC. Additionally, a diffuse structure near the Fermi level survives just above TC. Such behavior is well described by Monte Carlo simulations of a Kondo lattice model, thus supporting the formation of magnetic polarons in EuB6, which accounts for the resistivity upturn near above TC when lowering the temperature.

cond-mat.str-el↗

arXiv2020

Time-resolved resonant elastic soft X-ray scattering at Pohang Accelerator Laboratory X-ray Free Electron Laser

Resonant elastic X-ray scattering has been widely employed for exploring complex electronic ordering phenomena, like charge, spin, and orbital order, in particular in strongly correlated electronic systems. In addition, recent developments of pump-probe X-ray scattering allow us to expand the investigation of the temporal dynamics of such orders. Here, we introduce a new time-resolved Resonant Soft X-ray Scattering (tr-RSXS) endstation developed at the Pohang Accelerator Laboratory X-ray Free Electron Laser (PAL-XFEL). This endstation has an optical laser (wavelength of 800 nm plus harmonics) as the pump source. Based on the commissioning results, the tr-RSXS at PAL-XFEL can deliver a soft X-ray probe (400-1300 eV) with a time resolution about ~100 fs without jitter correction. As an example, the temporal dynamics of a charge density wave on a high-temperature cuprate superconductor is demonstrated.

physics.ins-det↗

arXiv2017

Electronic Structure Change of NiS$_{2-x}$Se$_x$ in the Metal-Insulator Transition Probed by X-ray Absorption Spectroscopy

The electronic structure change of NiS$_{2-x}$Se$_x$ as a function of Se concentration $x$ has been studied by Ni $L$-edge X-ray absorption spectroscopy (XAS). The XAS spectra show distinct features in Ni $L_3$ edge, indicating whether the system is insulating or metallic. These features can be semi-quantitatively explained within the framework of the configurational interaction cluster model (CICM). In the S-rich region, relatively large charge-transfer energy ($Δ\sim 5$ eV) from ligand $p$ to Ni 3$d$ states and a little small $p$-$d$ hybridization strength ($V_{pdσ} \sim 1.1$ eV) can reproduce the experimental spectra in the CICM calculation, and vice versa in the Se-rich region. Our analysis result is consistent with the Zaanen-Sawatzky-Allen scheme that the systems in S-rich side ($x \leq$ 0.5) are a charge transfer insulator. However, it also requires that the $Δ$ value must change abruptly in spite of the small change of $x$ near $x$=0.5. As a possible microscopic origin, we propose a percolation scenario where a long range connection of Ni[(S,Se)$_2$]$_6$ octahedra with Se-Se dimers plays a key role to gap closure.

cond-mat.str-el↗

arXiv2017

Charge-spin correlation in van der Waals antiferromagenet NiPS3

Strong charge-spin coupling is found in a layered transition-metal trichalcogenide NiPS3, a van derWaals antiferromagnet, from our study of the electronic structure using several experimental and theoretical tools: spectroscopic ellipsometry, x-ray absorption and photoemission spectroscopy, and density-functional calculations. NiPS3 displays an anomalous shift in the optical spectral weight at the magnetic ordering temperature, reflecting a strong coupling between the electronic and magnetic structures. X-ray absorption, photoemission and optical spectra support a self-doped ground state in NiPS3. Our work demonstrates that layered transition-metal trichalcogenide magnets are a useful candidate for the study of correlated-electron physics in two-dimensional magnetic material.

cond-mat.str-el↗

arXiv2017

Element-Specific Orbital Character in a Nearly-Free-Electron Superconductor Ag$_5$Pb$_2$O$_6$ Revealed by Core-Level Photoemission

Ag$_5$Pb$_2$O$_6$ has attracted considerable attention due to its novel nearly-free-electron superconductivity, but its electronic structure and orbital character of the Cooper-pair electrons remain controversial. Here, we present a method utilizing core-level photoemission to show that Pb 6$s$ electrons dominate near the Fermi level. We observe a strongly asymmetric Pb 4$f_{7/2}$ core-level spectrum, while a Ag 3$d_{5/2}$ spectrum is well explained by two symmetric peaks. The asymmetry in the Pb 4$f_{7/2}$ spectrum originates from the local attractive interaction between conducting Pb 6$s$ electrons and a Pb 4$f_{7/2}$ core hole, which implies a dominant Pb 6$s$ contribution to the metallic conduction. In addition, the observed Pb 4$f_{7/2}$ spectrum is not explained by the well-known Doniach-Šunjić lineshape for a simple metal. The spectrum is successfully generated by employing a Pb 6$s$ partial density of states from local density approximation calculations, thus confirming the Pb 6$s$ dominant character and free-electron-like density of states of Ag$_5$Pb$_2$O$_6$.

cond-mat.supr-con↗

arXiv2016

Electronic Structure of the Kitaev Material $α$-$\textrm{RuCl}_3$ Probed by Photoemission and Inverse Photoemission Spectroscopies

Recently, $α$-$\textrm{RuCl}_3$ has attracted much attention as a possible material realization of the honeycomb Kitaev model, which may stabilize a quantum-spin-liquid state. Compared to extensive studies on its magnetic properties, there is still a lack of understanding on its electronic structure, which is strongly related with its Kitaev physics. Here, the electronic structure of $α$-$\textrm{RuCl}_3$ is investigated by photoemission (PE) and inverse photoemission (IPE) spectroscopies. The band gap, directly measured from PE/IPE spectra, is found to be 1.9 eV, much larger than previous estimations. The LDA calculations show that the on-site Coulomb interaction $\textit{U}$ can open the band gap without spin-orbit coupling (SOC). However, the SOC should also be incorporated to reproduce the proper gap size, indicating that the interplay between $\textit{U}$ and SOC plays an essential role in the physics of $α$-$\textrm{RuCl}_3$. There exist some spectral features in PE/IPE spectra which cannot be explained by the LDA calculations. To explain such discrepancies, we perform the configuration-interaction calculations for a ${\textrm{RuCl}}_6^{3-}$ cluster. The experimental data and calculations demonstrate that the 4$\textit{d}$ compound $α$-$\textrm{RuCl}_3$ is a $J_{\textrm{eff}}$ = 1/2 Mott insulator rather than a quasimolecular-orbital insulator. Our study also provides important physical parameters, required in verifying the proposed Kitaev physics in $α$-$\textrm{RuCl}_3$.

cond-mat.str-el↗

arXiv2015

Latent Instabilities in Metallic LaNiO3 Films by Strain Control of Fermi-Surface Topology

Strain control is one of the most promising avenues to search for new emergent phenomena in transition-metal-oxide films. Here, we investigate the strain-induced changes of electronic structures in strongly correlated LaNiO3 (LNO) films, using angle-resolved photoemission spectroscopy and the dynamical mean-field theory. The strongly renormalized eg-orbital bands are systematically rearranged by misfit strain to change its fermiology. As tensile strain increases, the hole pocket centered at the A point elongates along the kz-axis and seems to become open, thus changing Fermi-surface (FS) topology from three- to quasi-two-dimensional. Concomitantly, the FS shape becomes flattened to enhance FS nesting. A FS superstructure with Q1 = (1/2,1/2,1/2) appears in all LNO films, while a tensile-strained LNO film has an additional Q2 = (1/4,1/4,1/4) modulation, indicating that some instabilities are present in metallic LNO films. Charge disproportionation and spin-density-wave fluctuations observed in other nickelates might be their most probable origins.

cond-mat.str-el↗

arXiv2014

Controlling the 2DEG states evolution at a metal/Bi$_2$Se$_3$ interface

We have demonstrated that the evolution of the two-dimensional electron gas (2DEG) system at an interface of metal and the model topological insulator (TI) Bi$_2$Se$_3$ can be controlled by choosing an appropriate kind of metal elements and by applying a low temperature evaporation procedure. In particular, we have found that only topological surface states (TSSs) can exist at a Mn/Bi$_2$Se$_3$ interface, which would be useful for implementing an electric contact with surface current channels only. The existence of the TSSs alone at the interface was confirmed by angle-resolved photoemission spectroscopy (ARPES). Based on the ARPES and core-level x-ray photoemission spectroscopy measurements, we propose a cation intercalation model to explain our findings.

cond-mat.mtrl-sci↗

arXiv2013

Dimensional crossover of the electronic structure in LaNiO3 ultrathin films: Orbital reconstruction, Fermi surface nesting, and the origin of the metal-insulator transition

Dimensionality control in the LaNiO3 (LNO) heterostructure has attracted attention due to its two-dimensional (2D) electronic structure was predicted to have an orbital ordered insulating ground state, analogous to that of the parent compound of high-Tc cuprate superconductors [P. Hansmann et al., Phys. Rev. Lett. 103, 016401 (2009)]. Here, we directly measured the electronic structure of LNO ultrathin films using in situ angle-resolved photoemission spectroscopy (ARPES). We recognized the dimensional crossover of the electronic structure around 3-unit cells (UC)-thick LNO film and observed the orbital reconstruction. However, complete orbital ordering was not achieved. Instead, we observed that the Fermi surface nesting effect became strong in the 2D LNO ultrathin film. These results indicated that the orbital reconstruction should be described by taking into account the strong nesting effect to search for the novel phenomena, such as superconductivity in 2D LNO heterostructure. In addition, the APRES spectra showed that the Fermi surface existed down to a 1-UC-thick film, which showed insulating behavior in transport measurements. We suggested that the metal-insulator transition in the transport properties may originate from Anderson localization.

cond-mat.str-el↗

arXiv2013

Thermoelectric imaging of structural disorder in epitaxial graphene

Heat is a familiar form of energy transported from a hot side to a colder side of an object, but not a notion associated with microscopic measurements of electronic properties. A temperature difference within a material causes charge carriers, electrons or holes, to diffuse along the temperature gradient inducing a thermoelectric voltage. Here we show that local thermoelectric measurements can yield high sensitivity imaging of structural disorder on the atomic and nanometre scales. The thermopower measurement acts to amplify the variations in the local density of states at the Fermi-level, giving high differential contrast in thermoelectric signals. Using this imaging technique, we uncovered point defects in the first layer of epitaxial graphene, which generate soliton-like domain wall line patterns separating regions of the different interlayer stacking of the second graphene layer.

cond-mat.mtrl-sci↗

arXiv2004

Core-Level X-Ray Photoemission Satellites in Ruthenates: A New Mechanism Revealing the Mott Transition

Ru 3d core-level x-ray photoemission spectra of various ruthenates are examined. They show in general two-peak structures, which can be assigned as the screened and unscreened peaks. The screened peak is absent in a Mott insulator, but develops into a main peak in the metallic regime. This spectral behavior is well explained by the dynamical mean-field theory calculation for the single-band Hubbard model with on-site core-hole potential using the exact diagonalization method. The new mechanism of the core-level photoemission satellite can be utilized to reveal the Mott transition phenomenon in various strongly correlated electron systems, especially in nano-scale devices and phase-separated materials.

cond-mat.str-el↗

arXiv2003

Localized Character of 4f Electrons in CeRh$_x$(x=2,3) and CeNi$_x$(x=2,5)

We have measured Ce 4f spectral weights of extremely $α$-like Ce-transition metal intermetallic compounds CeRh$_x$ (x=2,3) and CeNi$_x$ (x=2,5) by using the {\it bulk-sensitive} resonant photoemission technique at the Ce $M_5$($3d_{5/2}\to4f$)-edge. Unprecedentedly high energy resolution and longer escape depth of photoemitted electron at this photon energy enabled us to distinguish the sharp Kondo resonance tails at the Fermi level, which can be well described by the Gunnarsson-Schönhammer(GS) calculation based on the Anderson Impurity Hamiltonian. On the other hand, the itinerant 4f band description shows big discrepancies, which implies that Ce 4f electrons retain localized characters even in extremely $α$-like compounds.

cond-mat.str-el↗