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Changhee Sohn

Publications and source records attributed to Changhee Sohn.

At least 19 recordsLinked to original sources

Anomalous stabilization of excitons by metallic proximity

Metallic environments are generally expected to suppress excitons through strong dielectric screening, yet their influence can differ in composite systems where metallic and insulating regions coexist. Here, we investigate excitonic states in PdxCu1-xCrO2 thin films across a percolation-driven metal-insulator transition. Optical spectroscopy and many-body GW calculations show that CuCrO2 hosts strongly bound excitons with a binding energy of about 489 meV. With increasing Pd substitution, the system approaches an insulator-to-metal transition near x = 0.5, consistent with the site-percolation threshold of a triangular lattice. In the pre-percolation regime, the excitonic resonance redshifts by 241 meV while the Tanguy continuum onset remains nearly unchanged, consistent with a substantial increase in exciton binding energy before metallization. An image-charge-based excitonic hydrogen model shows that isolated metallic regions can enhance electron-hole binding through image-charge interactions, whereas conventional screening is recovered once a continuous metallic network forms. Although this model provides a possible interpretation of the observed excitonic evolution, an alternative scenario in which metallic and excitonic responses originate from electronically distinct states and evolve independently cannot be excluded. These results reveal unusual metallic-excitonic coexistence near a percolation-driven metal-insulator transition and suggest nanoscale metallic proximity as a possible route for modifying excitonic interactions.

cond-mat.str-el

$p$-wave magnet and hedgehog-type Berry curvature in helimagnetic MnAu$_2$

Recently discovered altermagnetism in collinear compensated magnets shows even-parity spin texture in momentum space. Beyond the collinear spin ordering, unique odd-parity spin textures emerge in noncollinear compensated magnets. The noncollinear candidates, however, remain unexplored toward a room-temperature metallic altermagnet. Here, we demonstrate that MnAu2 exhibits metallic p-wave magnetism and large spin splitting induced by helical spin ordering. By adapting the band-unfolding scheme based on the translation operators combined with spin rotations, first-principles calculations reveal an unconventional Fermi surface around the $\tilde{M}$-point composed of a single electron pocket with $p$-wave spin texture. Moreover, the spin twist in the helimagnet triggers topologically non-trivial hedgehog Berry curvature, which links to the nonlinear Hall effect and spin Hall effect. Considering the experimental T$_C$ = 335 to 370 K, MnAu$_2$ could establish itself as an ideal candidate for a room-temperature metallic $p$-wave magnet, promising for versatile spintronic applications.

cond-mat.mtrl-sci

Ferroelectric amplitude switching and continuous memory

Although ferroelectric systems inherently exhibit binary switching behavior, recent advances in analog memory device have spurred growing interest in achieving continuous memory states. In this work, we demonstrate ferroelectric amplitude switching at the mesoscopic scale in compositionally graded Ba1-xSrxTiO3 heterostructures, enabling continuous modulation of polarization magnitude without altering its direction, which we defined as amplitude switching. Using switching current measurement, piezoresponse force microscopy and Landau-Ginzburg-Devonshire simulations, we reveal that compositionally graded ferroelectric heterostructure can possess amplitude switching behavior through a double well potential with flattened minima. This behavior supports stable, continuous polarization states and establishes a new platform for analog memory applications. These findings introduce amplitude switching as a new dynamic of the order parameter, paving the way for energy-efficient and reliable analog memory systems.

cond-mat.mtrl-sci

Tunneling magnetoresistance in altermagnetic RuO$_2$-based magnetic tunnel junctions

Altermagnets exhibit characteristics akin to antiferromagnets, with spin-split anisotropic bands in momentum space. RuO$_2$ has been considered as a prototype altermagnet; however, recent reports have questioned altermagnetic ground state in this material. In this study, we provide direct experimental evidence of altermagnetic characteristics in RuO$_2$ films by demonstrating spin-dependent tunneling magnetoresistance (TMR) in RuO$_2$-based magnetic tunnel junctions. Our results show the spin-splitted anisotropic band structure of RuO$_2$, with the observed TMR determined by the direction of the N\'eel vector of RuO$_2$. These results reflect the altermagnetic nature of RuO$_2$ and highlight its potential for spintronic applications, leveraging the combined strengths of ferromagnetic and antiferromagnetic systems.

cond-mat.mtrl-sci

Colossal optical anisotropy in wide-bandgap semiconductor CuAlO2

Colossal optical anisotropy in the entire visible spectrum is crucial for advanced photonic applications, enabling precise light manipulation without optical loss across a broad spectral range. Here, we demonstrate that CuAlO2 exhibits colossal optical anisotropy and transparency across the visible spectrum, enabled by its unique three-dimensional O-Cu-O dumbbell structure and two-dimensionally confined excitons. Using mm-sized single crystals, we independently measured ab-plane and c-axis optical properties, revealing maximum birefringence (= 3.67) and linear dichroism (= 5.21), the highest reported to date. CuAlO2 retains birefringence over 0.5 throughout the entire visible range and possesses a wide direct bandgap of 3.71 eV, surpassing the birefringence of commercial anisotropic crystals transparent in the visible spectrum. From the two-dimensional screened hydrogen model and first-principles calculations, we demonstrate that the colossal anisotropy arises from a unique excitonic Cu d-p transition confined to the atomic-thick layer. This colossal optical anisotropy and transparency across the entire visible spectrum makes CuAlO2 a promising candidate for future photonic technologies.

cond-mat.mtrl-sci

Nanoscale magnetic ordering dynamics in a high Curie temperature ferromagnet

Thermally driven transitions between ferromagnetic and paramagnetic phases are characterized by critical behavior with divergent susceptibilities, long-range correlations, and spin dynamics that can span kHz to GHz scales as the material approaches the critical temperature $\mathrm{T_c}$, but it has proven technically challenging to probe the relevant length and time scales with most conventional measurement techniques. In this study, we employ scanning nitrogen-vacancy center based magnetometry and relaxometry to reveal the critical behavior of a high-$\mathrm{T_c}$ ferromagnetic oxide near its Curie temperature. Cluster analysis of the measured temperature-dependent nanoscale magnetic textures points to a 3D universality class with a correlation length that diverges near $\mathrm{T_c}$. Meanwhile, the temperature-dependent spin dynamics, measured through all optical relaxometry suggest that the phase transition is in the XY universality class. Our results capture both static and dynamic aspects of critical behavior, providing insights into universal properties that govern phase transitions in magnetic materials.

cond-mat.mtrl-sci

Suppression of Antiferromagnetic Order by Strain in Honeycomb Cobaltate: Implication for Quantum Spin Liquid

Recently, layered honeycomb cobaltates have been predicted as a new promising system for realizing the Kitaev quantum spin liquid, a many-body quantum entangled ground state characterized by fractional excitations. However, these cobaltates, similar to other candidate materials, exhibit classical antiferromagnetic ordering at low temperatures, which impedes the formation of the expected quantum state. Here, we demonstrate that the control of the trigonal crystal field of Co ions is crucial to suppress classical antiferromagnetic ordering and to locate its ground state in closer vicinity to quantum spin liquid in layered honeycomb cobaltates. By utilizing heterostructure engineering on Cu3Co2SbO6 thin films, we adjust the trigonal distortion of CoO6 octahedra and the associated trigonal crystal field. The original N\'eel temperature of 16 K in bulk Cu3Co2SbO6 decreases (increases) to 7.8 K (22.7 K) in strained Cu3Co2SbO6 films by decreasing (increasing) the magnitude of the trigonal crystal fields. Our experimental finding substantiates the potential of layered honeycomb cobaltate heterostructures and strain engineering to accomplish the extremely elusive quantum phase of matter.

cond-mat.str-el

Optical detection of bond-dependent and frustrated spin in the two-dimensional cobalt-based honeycomb antiferromagnet Cu3Co2SbO6

Two-dimensional honeycomb antiferromagnet becomes an important class of materials as it can provide a route to Kitaev quantum spin liquid, characterized by massive quantum entanglement and fractional excitations. The signatures of its proximity to Kitaev quantum spin liquid in the honeycomb antiferromagnet includes anisotropic bond-dependent magnetic responses and persistent fluctuation by frustration in paramagnetic regime. Here, we propose Cu3Co2SbO6 heterostructures as an intriguing honeycomb antiferromagnet for quantum spin liquid, wherein bond-dependent and frustrated spins interact with optical excitons. This system exhibits antiferromagnetism at 16 K with different spin-flip magnetic fields between a bond-parallel and bond-perpendicular directions, aligning more closely with the generalized Heisenberg-Kitaev than the XXZ model. Optical spectroscopy reveals a strong excitonic transition coupled to the antiferromagnetism, enabling optical detection of its spin states. Particularly, such spin-exciton coupling presents anisotropic responses between bond-parallel and bond-perpendicular magnetic field as well as a finite spin-spin correlation function around 40 K, higher than twice its N\'eel temperature. The characteristic temperature that remains barely changed even under strong magnetic fields highlights the robustness of the spin-fluctuation region. Our results demonstrate Cu3Co2SbO6 as a unique candidate for the quantum spin liquid phase, where the spin Hamiltonian and quasiparticle excitations can be probed and potentially controlled by light.

cond-mat.str-el

Structural Anisotropy in Sb Thin Films

Sb thin films have attracted wide interests due to their tunable band structure, topological phases, and remarkable electronic properties. We successfully grow epitaxial Sb thin films on a closely lattice-matched GaSb(001) surface by molecular beam epitaxy. We find a novel anisotropic directional dependence of their structural, morphological, and electronic properties. The origin of the anisotropic features is elucidated using first-principles density functional theory (DFT) calculations. The growth regime of crystalline and amorphous Sb thin films was determined by mapping the surface reconstruction phase diagram of the GaSb(001) surface under Sb$_2$ flux, with confirmation of structural characterizations. Crystalline Sb thin films show a rhombohedral crystal structure along the rhombohedral (104) surface orientation parallel to the cubic (001) surface orientation of the GaSb substrate. At this coherent interface, Sb atoms are aligned with the GaSb lattice along the [1-10] crystallographic direction but are not aligned well along the [110] crystallographic direction, which results in anisotropic features in reflection high-energy electron diffraction patterns, surface morphology, and transport properties. Our DFT calculations show that the anisotropic features originate from the GaSb surface, where Sb atoms align with the Ga and Sb atoms on the reconstructed surface. The formation energy calculations confirm that the stability of the experimentally observed structures. Our results provide optimal film growth conditions for further studies of novel properties of Bi$_{1-x}$Sb$_x$ thin films with similar lattice parameters and an identical crystal structure as well as functional heterostructures of them with III-V semiconductor layers along the (001) surface orientation, supported by a theoretical understanding of the anisotropic film orientation.

cond-mat.mtrl-sci

Honeycomb oxide heterostructure: a new platform for Kitaev quantum spin liquid

Kitaev quantum spin liquid, massively quantum entangled states, is so scarce in nature that searching for new candidate systems remains a great challenge. Honeycomb heterostructure could be a promising route to realize and utilize such an exotic quantum phase by providing additional controllability of Hamiltonian and device compatibility, respectively. Here, we provide epitaxial honeycomb oxide thin film Na3Co2SbO6, a candidate of Kitaev quantum spin liquid proposed recently. We found a spin glass and antiferromagnetic ground states depending on Na stoichiometry, signifying not only the importance of Na vacancy control but also strong frustration in Na3Co2SbO6. Despite its classical ground state, the field-dependent magnetic susceptibility shows remarkable scaling collapse with a single critical exponent, which can be interpreted as evidence of quantum criticality. Its electronic ground state and derived spin Hamiltonian from spectroscopies are consistent with the predicted Kitaev model. Our work provides a unique route to the realization and utilization of Kitaev quantum spin liquid.

cond-mat.str-el

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

Reversibly controlled ternary polar states and ferroelectric bias promoted by boosting square-tensile-strain

Interaction between dipoles often emerges intriguing physical phenomena, such as exchange bias in the magnetic heterostructures and magnetoelectric effect in multiferroics, which lead to advances in multifunctional heterostructures. However, the defect-dipole tends to be considered the undesired to deteriorate the electronic functionality. Here, we report deterministic switching between the ferroelectric and the pinched states by exploiting a new substrate of cubic perovskite, BaZrO$_{3}$, which boosts square-tensile-strain to BaTiO$_{3}$ and promotes four-variants in-plane spontaneous polarization with oxygen vacancy creation. First-principles calculations propose a complex of an oxygen vacancy and two Ti$^{3+}$ ions coins a charge-neutral defect-dipole. Cooperative control of the defect-dipole and the spontaneous polarization reveals ternary in-plane polar states characterized by biased/pinched hysteresis loops. Furthermore, we experimentally demonstrate that three electrically controlled polar-ordering states lead to switchable and non-volatile dielectric states for application of non-destructive electro-dielectric memory. This discovery opens a new route to develop functional materials via manipulating defect-dipoles and offers a novel platform to advance heteroepitaxy beyond the prevalent perovskite substrates.

cond-mat.mtrl-sci

Preparation of large Cu3Sn single crystal by Czochralski method

Cu3Sn was recently predicted to host topological Dirac fermions, but related research is still in its infancy. The growth of large and high-quality Cu3Sn single crystals is, therefore, highly desired to investigate the possible topological properties. In this work, we report the single crystal growth of Cu3Sn by Czochralski (CZ) method. Crystal structure, chemical composition, and transport properties of Cu3Sn single crystals were analyzed to verify the crystal quality. Notably, compared to the mm-sized crystals from a molten Sn-flux, the cm-sized crystals obtained by the CZ method are free from contamination from flux materials, paving the way for the follow-up works.

cond-mat.mtrl-sci

Correlated Oxide Dirac Semimetal in the Extreme Quantum Limit

Quantum materials (QMs) with strong correlation and non-trivial topology are indispensable to next-generation information and computing technologies. Exploitation of topological band structure is an ideal starting point to realize correlated topological QMs. Herein, we report that strain-induced symmetry modification in correlated oxide SrNbO3 thin films creates an emerging topological band structure. Dirac electrons in strained SrNbO3 films reveal ultra-high mobility (100,000 cm2/Vs), exceptionally small effective mass (0.04me), and non-zero Berry phase. More importantly, strained SrNbO3 films reach the extreme quantum limit, exhibiting a sign of fractional occupation of Landau levels and giant mass enhancement. Our results suggest that symmetry-modified SrNbO3 is a rare example of a correlated topological QM, in which strong correlation of Dirac electrons leads to the realization of fractional occupation of Landau levels.

cond-mat.str-el

Pulsed-laser epitaxy of metallic delafossite PdCrO$_2$ films

Alternate stacking of a highly conducting metallic layer with a magnetic triangular layer found in delafossite PdCrO2 provides an excellent platform for discovering intriguing correlated quantum phenomena. Thin film growth of the material may enable not only tuning the basic physical properties beyond what bulk materials can exhibit, but also developing novel hybrid materials by interfacing with dissimilar materials, yet this has proven to be extremely challenging. Here, we report the epitaxial growth of metallic delafossite PdCrO2 films by pulsed laser epitaxy (PLE). The fundamental role of the PLE growth conditions, epitaxial strain, and chemical and structural characteristics of the substrate is investigated by growing under various growth conditions and on various types of substrates. While strain plays a large role in improving the crystallinities, the direct growth of epitaxial PdCrO2 films without impurity phases was not successful. We attribute this difficulty to both the chemical and structural dissimilarities between the substrates and volatile nature of PdO layer, which make nucleation of the right phase difficult. This difficulty was overcome by growing CuCrO2 buffer layers before PdCrO2 were grown. Unlike PdCrO2, CuCrO2 films were rather readily grown with a relatively wide growth window. Only monolayer thick buffer layer was sufficient to grow the correct PdCrO2 phase. This result indicates that the epitaxy of Pd-based delafossites is extremely sensitive to the chemistry and structure of the interface, necessitating near perfect substrate materials. The resulting films are commensurately strained and show an antiferromagnetic transition at 40 K that persists down to as thin as 3.6 nm in thickness.

physics.app-ph

Doped NiO: the Mottness of a charge transfer insulator

The evolution of the electronic structures of strongly correlated insulators with doping has long been a central fundamental question in condensed matter physics; it is also of great practical relevance for applications. We have studied the evolution of NiO under hole {\em and} electron doping using high-quality thin film and a wide range of experimental and theoretical methods. The evolution is in both cases very smooth with dopant concentration. The band gap is asymmetric under electron and hole doping, consistent with a charge-transfer insulator picture, and is reduced faster under hole than electron doping. For both electron and hole doping, occupied states are introduced at the top of the valence band. The formation of deep donor levels under electron doping and the inability to pin otherwise empty states near the conduction band edge is indicative that local electron addition and removal energies are dominated by a Mott-like Hubbard $U$-interaction even though the global bandgap is predominantly a charge-transfer type gap.

cond-mat.str-el

Reflection anisotropy experiments to study non-equilibrium dynamics of electronic nematicity

Electronic nematicity have attracted a great deal of interest in the unconventional superconductivity research. We present an experimental method to investigate reflectivity anisotropy by the electronic nematicity and its non-equilibrium dynamics. Our experimental results on Ba(Fe$_{0.955}$Co$_{0.045}$)$_{2}$As$_{2}$ single crystal clearly feature the broken four-fold symmetry along directions parallel to Fe-Fe bonding. Numerical simulations using WVASE from Woollam Co. demonstrate that our method is highly reliable under various experimental conditions. Finally, we perform time-resolved reflectivity anisotropy measurement confirming that photo-excitation by 1.55 eV photons suppresses the reflectivity anisotropy due to nematic order.

physics.optics

Competing Phases in Epitaxial Vanadium Dioxide at Nanoscale

Phase competition in correlated oxides offers tantalizing opportunities as many intriguing physical phenomena occur near the phase transitions. Owing to a sharp metal-insulator transition (MIT) near room temperature, correlated vanadium dioxide (VO2) exhibits a strong competition between insulating and metallic phases that is important for practical applications. However, the phase boundary undergoes strong modification when strain is involved, yielding complex phase transitions. Here, we report the emergence of the nanoscale M2 phase domains in VO2 epitaxial films under anisotropic strain relaxation. The phase states of the films are imaged by multi-length-scale probes, detecting the structural and electrical properties in individual local domains. Competing evolution of the M1 and M2 phases indicates a critical role of lattice-strain on both the stability of the M2 Mott phase and the energetics of the MIT in VO2 films. This study demonstrates how strain engineering can be utilized to design phase states, which allow deliberate control of MIT behavior at the nanoscale in epitaxial VO2 films.

cond-mat.str-el