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Choongjae Won

Publications and source records attributed to Choongjae Won.

15 recordsLinked to original sources

Giant spontaneous Kerr effect and its self-doping dependence in altermagnetic MnTe

Altermagnetism, a third class of collinear magnetism with spin-split bands and vanishing net magnetization, has emerged in hexagonal {\alpha}-MnTe, a promising platform for ultrafast, stray-field-free spintronics. Whether MnTe's macroscopic symmetry-breaking signatures reflect ideal altermagnetic order or are activated by defects remains open. Here we report giant spontaneous Kerr rotations of up to 1500 rad in {\alpha}-MnTe single crystals at the telecommunication wavelength of 1550 nm, onsetting precisely at the N\'eel temperature TN = 307 K. The signal appears in disjoint macroscopic patches whose amplitude tracks the sample conductivity, and a hole-conducting {\alpha}-MnTe film reproduces this response together with an anomalous Hall effect. Within a single crystal, Kerr-active regions are optically distinct from their Kerr-silent surroundings in co-registered reflection maps. These observations indicate that carrier self-doping, rather than ideal altermagnetic order alone, governs the giant magneto-optical response, and establish telecom-wavelength Kerr imaging as a practical readout for altermagnetic spintronics.

cond-mat.str-el

X-ray magnetic circular dichroism evidence of intrinsic $d$-wave altermagnetism in rutile-structure NiF$_2$

We present the x-ray magnetic circular dichroism (XMCD) at the Ni $L_{2,3}$-edge as an evidence of the $d$-wave altermagnetism in rutile-structure NiF$_2$. Sizable XMCD signal is observed in excellent agreement with theoretical simulations. Owing to a considerable net magnetization due to spin canting, the XMCD spectrum consists of an altermagnetic signal as well as a non-negligible ferromagnetic contribution. We verify experimentally that the XMCD spectrum can be written as a sum of contributions from altermagnetism and weak ferromagnetism. Two experimental methods to isolate the ferromagnetic contribution are shown to yield essentially the same result. These are dependence of XMCD on applied magnetic fields below the Néel temperature and the XMCD measured in applied field above the Néel temperature. Our results demonstrate the utility of XMCD as a probe for altermagnetic materials with the coexisting weak ferromagnetism induced by the relativistic spin-orbit coupling.

cond-mat.str-el

Exciton photoemission from a ground state of a solid Ta2Pd3Te5

Excitons are bosonic quasiparticles with a variety of applications in optoelectronics, photosyn thesis, and dissipationless informatics, and their lifetime can become sufficiently long to form a quantum condensate. While exciton condensation has been predicted to occur as a ground state of a solid, so called an excitonic insulator, whose material realization has been elusive. Here we report the observation of direct photoemission signals from excitons in a ground state of a very recent excitonic insulator candidate Ta2Pd3Te5 below its metal-insulator transition temperature using orbital-selective angle-resolved photoemission spectroscopy. It is confirmed that the excitons have a lower energy than the valence band maximum to possibly drive the phase transition. This measurement further discloses the size and the unusual odd parity of the exciton wave function. The present finding opens an avenue toward applications of coherent excitons in solid systems and searching for exotic quantum phases of exciton condensates.

cond-mat.str-el

Time-domain decoding of unconventional charge order mechanisms in nonmagnetic and magnetic kagome metals

In kagome lattice materials, quantum interplay between charge, spin, orbital, and lattice degrees of freedom gives rise to a remarkably rich set of emergent phenomena, ranging from unconventional charge order and superconductivity to topological magnetism. While the exact nature of these exotic orders is often challenging to comprehend in static experiments, time-resolved techniques can offer critical insights by disentangling coupled degrees of freedom on the time-axis. In this work, we demonstrate that the nature of charge orders in two representative kagome metals - nonmagnetic ScV6Sn6 and magnetic FeGe - which has been highly controversial in static studies, can be directly deciphered in the time-domain through their fundamentally distinct order parameter dynamics measured via time-resolved X-ray scattering at an X-ray free electron laser. In nonmagnetic ScV6Sn6, the dynamics are characterized by ultrafast melting and coherent amplitudon oscillations, typical of a phonon-coupled charge order. In stark contrast, magnetic FeGe exhibits resilient metastable charge order dynamics, hitherto unobserved in any other charge-ordered system - this unique time-domain behavior directly signifies an unconventional magnetism-interlocked charge order state realized in this kagome magnet. Our results not only provide a model case where unconventional nature of electronic order, hidden in equilibrium, is directly unraveled in the time-domain, but also pave the way for future out-of-equilibrium engineering of novel quantum orders in kagome lattice platforms.

cond-mat.str-el

Frustrated phonon with charge density wave in vanadium Kagome metal

The formation of a star of David CDW superstructure, resulting from the coordinated displacements of vanadium ions on a corner sharing triangular lattice, has garnered significant attention to comprehend the influence of electron phonon interaction within geometrically intricate lattice of Kagome metals, specifically AV3Sb5 (where A represents K, Rb, or Cs). However, understanding of the underlying mechanism behind CDW formation, coupled with symmetry protected lattice vibrations, remains elusive. Here, from femtosecond time resolved X ray scattering experiments, we reveal that the phonon mode, associated with Cs ions out-of-plane motion, becomes frustrated in the CDW phase. Furthermore, we observed the photoinduced emergence of a metastable CDW phase, facilitated by alleviating the frustration. By not only elucidating the longstanding puzzle surrounding the intervention of phonons but introducing the phononic frustration, this research offers fresh insights into the competition between phonons and periodic lattice distortions, a phenomenon widespread in other correlated quantum materials including layered high TC superconductors.

cond-mat.str-el

Spin Excitation Continuum in the Exactly Solvable Triangular-Lattice Spin Liquid CeMgAl11O19

In magnetically ordered insulators, elementary quasiparticles manifest as spin waves - collective motions of localized magnetic moments propagating through the lattice - observed via inelastic neutron scattering. In effective spin-1/2 systems where geometric frustrations suppress static magnetic order, spin excitation continua can emerge, either from degenerate classical spin ground states or from entangled quantum spins characterized by emergent gauge fields and deconfined fractionalized excitations. Comparing the spin Hamiltonian with theoretical models can unveil the microscopic origins of these zero-field spin excitation continua. Here, we use neutron scattering to study spin excitations of the two-dimensional (2D) triangular-lattice effective spin-1/2 antiferromagnet CeMgAl11O19. Analyzing the spin waves in the field-polarized ferromagnetic state, we find that the spin Hamiltonian is close to an exactly solvable 2D triangular-lattice XXZ model, where degenerate 120$^\circ$ ordered ground states - umbrella states - develop in the zero temperature limit. We then find that the observed zero-field spin excitation continuum matches the calculated ensemble of spin waves from the umbrella state manifold, and thus conclude that CeMgAl11O19 is the first example of an exactly solvable spin liquid on a triangular lattice where the spin excitation continuum arises from the ground state degeneracy.

cond-mat.str-el

Kibble-Zurek mechanism of Ising domains

The formation of topological defects after a symmetry-breaking phase transition is an overarching phenomenon that encodes rich information about the underlying dynamics. Kibble-Zurek mechanism (KZM), which describes these nonequilibrium dynamics, predicts defect densities of these second-order phase transitions driven by thermal fluctuations. It has been verified as a successful model in a wide variety of physical systems, finding applications from structure formation in the early universe to condensed matter systems. However, whether topologically-trivial Ising domains, one of the most common and fundamental types of domains in condensed matter systems, also obey the KZM has never been investigated in the laboratory. We examined two different kinds of three-dimensional (3D) structural Ising domains: clockwise (CW)/counter-clockwise (CCW) ferro-rotation domains in NiTiO3 and up/down polar domains in BiTeI. While the KZM slope of ferro-rotation domains in NiTiO3 agrees well with the prediction of the 3D Ising model, the KZM slope of polar domains in BiTeI surprisingly far exceeds the theoretical limit, setting an exotic example where possible weak long-range dipolar interactions play a critical role in steepening the KZM slope of non-topological quantities. Our results demonstrate the validity of KZM for Ising domains and reveal an enhancement of the power-law exponent and a possible reduction of the dynamic critical exponent z for transitions with long-range interactions.

cond-mat.stat-mech

Kinkless electronic junction along one dimensional electronic channel

Here we report the formation of type-A and type-B electronic junctions without any structural discontinuity along a well-defined 1-nm-wide one-dimensional electronic channel within a van der Waals layer. We employ scanning tunneling microscopy and spectroscopy techniques to investigate the atomic and electronic structure along peculiar domain walls formed on the charge-density-wave phase of 1T-TaS2. We find distinct kinds of abrupt electronic junctions with discontinuities of the band gap along the domain walls, which do not have any structural kinks and defects. Our density-functional calculations reveal a novel mechanism of the electronic junction formation; they are formed by a kinked domain wall in the layer underneath through substantial electronic interlayer coupling. This work demonstrates that the interlayer electronic coupling can be an effective control knob over several-nanometer-scale electronic property of two-dimensional atomic monolayers.

cond-mat.str-el

Nature of charge density wave in kagome metal ScV6Sn6

Kagome lattice materials offer a fertile ground to discover novel quantum phases of matter, ranging from unconventional superconductivity and quantum spin liquids to charge orders of various profiles. However, understanding the genuine origin of the quantum phases in kagome materials is often challenging, owing to the intertwined atomic, electronic, and structural degrees of freedom. Here, we combine angle-resolved photoemission spectroscopy, phonon mode calculation, and chemical doping to elucidate the driving mechanism of the root3*root3 charge order in a newly discovered kagome metal ScV6Sn6. In contrast to the case of the archetype kagome system AV3Sb5 (A= K, Rb, Cs), the van Hove singularities in ScV6Sn6 remain intact across the charge order transition, indicating a marginal role of the electronic instability from the V kagome lattice. Instead, we identified a three-dimensional band with dominant planar Sn character opening a large charge order gap of 260 meV and strongly reconstructing the Fermi surface. Our complementary phonon dispersion calculations further emphasize the role of the structural components other than the V kagome lattice by revealing the unstable planar Sn and Sc phonon modes associated to the root3*root3 phase. Finally, in the constructed phase diagram of Sc(V1-xCrx)6Sn6, the charge order remains robust in a wide doping range x = 0 ~ 0.10 against the Fermi level shift up to ~ 120 meV, further making the electronic scenarios such as Fermi surface or saddle point nesting unlikely. Our multimodal investigations demonstrate that the physics of ScV6Sn6 is fundamentally different from the canonical kagome metal AV3Sb5, uncovering a new mechanism to induce symmetry-breaking phase transition in kagome lattice materials.

cond-mat.str-el

Topological Surface Magnetism and Neel Vector Control in a Magnetoelectric Antiferromagnet

Antiferromagnetic states with no stray magnetic fields can enable high-density ultra-fast spintronic technologies. However, the detection and control of antiferromagnetic Neel vectors remain challenging. Linear magnetoelectric antiferromagnets (LMAs) may provide new pathways, but applying simultaneous electric and magnetic fields, necessary to control Neel vectors in LMAs, is cumbersome and impractical for most applications. Herein, we show that Cr2O3, a prototypical room-temperature LMA, carries a topologically-protected surface magnetism in all surfaces, which stems from intrinsic surface electric fields due to band bending, combined with the bulk linear magnetoelectricity. Consequently, bulk Neel vectors with zero bulk magnetization can be simply tuned by magnetic fields through controlling the magnetizations associated with the surface magnetism. Our results imply that the surface magnetizations discovered in Cr2O3 should be also present in all LMAs.

cond-mat.mtrl-sci

Vibrational properties of CuInP2S6 across the ferroelectric transition

In order to explore the properties of a two-sublattice ferroelectric, we measured the infrared and Raman scattering response of CuInP2S6 across the ferroelectric and glassy transitions and compared our findings to a symmetry analysis, calculations of phase stability, and lattice dynamics. In addition to uncovering displacive character and a large hysteresis region surrounding the ferroelectric transition temperature T_C, we identify the vibrational modes that stabilize the polar phase and confirm the presence of two ferroelectric variants with opposite polarizations. Below TC, a poorly understood relaxational or glassy transition at Tg is characterized by local structure changes in the form of subtle peak shifting and activation of low frequency out-of-plane Cu- and In-containing modes. The latter are due to changes in the Cu/In coordination environments and associated order-disorder processes. Moreover, Tg takes place in two steps with another large hysteresis region and significant underlying scattering. Combined with imaging of the room temperature phase separation, this effort lays the groundwork for studying CuInP2S6 under external stimuli and in the ultra-thin limit.

cond-mat.mtrl-sci

Large Orbital Magnetic Moment and Strong Perpendicular Magnetic Anisotropy in Heavily Intercalated Fe$_{x}$TiS$_2$

Titanium disulfide TiS$_2$, which is a member of the layered transition-metal dichalcogenides with the 1T-CdI$_2$-type crystal structure, is known to exhibit a wide variety of magnetism through intercalating various kinds of transition-metal atoms of different concentrations. Among them, Fe-intercalated titanium disulfide Fe$_x$TiS$_2$ is known to be ferromagnetic with strong perpendicular magnetic anisotropy (PMA) and large coercive fields ($H_\text{c}$). In order to study the microscopic origin of the magnetism of this compound, we have performed X-ray absorption spectroscopy (XAS) and X-ray magnetic circular dichroism (XMCD) measurements on single crystals of heavily intercalated Fe$_x$TiS$_2$ ($x\sim0.5$). The grown single crystals showed a strong PMA with a large $H_\text{c}$ of $μ_0H_\text{c} \simeq 1.0\ \text{T}$. XAS and XMCD spectra showed that Fe is fully in the valence states of 2+ and that Ti is in an itinerant electronic state, indicating electron transfer from the intercalated Fe atoms to the host TiS$_2$ bands. The Fe$^{2+}$ ions were shown to have a large orbital magnetic moment of $\simeq 0.59\ μ_\text{B}\text{/Fe}$, to which, combined with the spin-orbit interaction and the trigonal crystal field, we attribute the strong magnetic anisotropy of Fe$_x$TiS$_2$.

cond-mat.mtrl-sci

Ultrafast Modulations And Detection of a Ferro-rotational Charge Density Wave Using Time-resolved Electric Quadrupole Second Harmonic Generation

We show the ferro-rotational nature of the commensurate charge density wave (CCDW) in $1T$-$\mathrm{TaS}_2$ and track its dynamic modulations by temperature-dependent and time-resolved electric quadrupole rotation anisotropy-second harmonic generation (EQ RA-SHG), respectively. The ultrafast modulations manifest as the breathing and the rotation of the EQ RA-SHG patterns at three frequencies around the reported single CCDW amplitude mode frequency. A sudden shift of the triplet frequencies and a dramatic increase in the breathing and rotation magnitude further reveal a photo-induced transient CDW phase across a critical pump fluence of ~ 0.5 mJ/cm$^2$.

cond-mat.mtrl-sci

Honeycomb-Lattice Mott insulator on Tantalum Disulphide

Effects of electron many-body interactions amplify in an electronic system with a narrow bandwidth opening a way to exotic physics. A narrow band in a two-dimensional (2D) honeycomb lattice is particularly intriguing as combined with Dirac bands and topological properties but the material realization of a strongly interacting honeycomb lattice described by the Kane-Mele-Hubbard model has not been identified. Here we report a novel approach to realize a 2D honeycomb-lattice narrow-band system with strongly interacting 5$d$ electrons. We engineer a well-known triangular lattice 2D Mott insulator 1T-TaS$_2$ into a honeycomb lattice utilizing an adsorbate superstructure. Potassium (K) adatoms at an optimum coverage deplete one-third of the unpaired $d$ electrons and the remaining electrons form a honeycomb lattice with a very small hopping. Ab initio calculations show extremely narrow Z$_2$ topological bands mimicking the Kane-Mele model. Electron spectroscopy detects an order of magnitude bigger charge gap confirming the substantial electron correlation as confirmed by dynamical mean field theory. It could be the first artificial Mott insulator with a finite spin Chern number.

cond-mat.str-el

Neutron Scattering Investigation of Rhenium Orbital Ordering in $3d-5d$ Double Perovskite Ca$_2$FeReO$_6$

We have carried out inelastic neutron scattering experiments to study magnetic excitations in ordered double perovskite Ca$_2$FeReO$_6$. We found a well-defined magnon mode with a bandwidth of $\sim$50meV below the ferri-magnetic ordering temperature ($T_c\sim$520K), similar to previously studied Ba$_2$FeReO$_6$. The spin excitation is gapless for most temperatures within the magnetically ordered phase. However, a spin gap of $\sim$10meV opens up below $\sim$150K, which is well below the magnetic ordering temperature but coincides with a previously reported metal-insulator transition and onset of structural distortion. The observed temperature dependence of spin gap provides strong evidence for ordering of Re orbitals at $\sim$150~K, in accordance with earlier proposal put forward by Oikawa $\it{et.\,al}$ based on neutron diffraction [J. Phys. Soc. Jpn., $\bf{72}$, 1411 (2003)] as well as recent theoretical work by Lee and Marianetti [Phys. Rev. B, $\bf{97}$, 045102 (2018)]. The presence of separate orbital and magnetic ordering in Ca$_2$FeReO$_6$ suggests weak coupling between spin and orbital degrees of freedom and hints towards a sub-dominant role played by spin orbit coupling in describing its magnetism. In addition, we observed only one well-defined magnon band near magnetic zone boundary, which is incompatible with simple ferrimagnetic spin waves arising from Fe and Re local moments, but suggests a strong damping of Re magnon mode.

cond-mat.str-el