arXiv subjects

In Hyeok Choi

Publications and source records attributed to In Hyeok Choi.

11 recordsLinked to original sources

arXiv2026

Terahertz two-dimensional coherent spectroscopy: unlocking coherent quantum intraband nonlinear dynamics

Quantum materials host a rich spectrum of low-energy collective excitations- phonons, magnons, plasmons, polaritons, and Higgs modes- that fundamentally govern their emergent properties, but remain inaccessible to conventional linear THz spectroscopy when nonlinear pathways overlap or non-perturbative dynamics emerge. Terahertz two-dimensional coherent spectroscopy (THz-2DCS), realized through phase-stable high-field THz pulse sequences, directly resolves this challenge by delivering phase-resolved multidimensional spectra that uniquely disentangle coherent intraband nonlinear quantum dynamics from incoherent backgrounds. Here, we establish a unified theoretical framework by using density-matrix formalism combined with the optical Bloch equations, from which nonlinear pathways are systematically derived and visualized on the Bloch sphere. This framework provides insight into low-energy nonlinear dynamics exhibiting homogeneous or inhomogeneous broadening depending on the scattering mechanism, enabling the interpretation of nonlinear signals in both the perturbative regime, described by a susceptibility expansion, and the non-perturbative regime. Building on this foundation, we comprehensively survey THz-2DCS investigations of nonlinear plasmon, phonon, magnon, and polariton. Finally, we outline future opportunities, including integration with optical-pump THz-probe platforms for nonequilibrium quantum control.

physics.optics↗

arXiv2026

Light-Driven Ultrafast Control of Time-Reversal Symmetry in SrTiO3

Light-driven control of material symmetry enables the engineering of phenomena forbidden in equilibrium. Although electromagnetic fields have been used to break time-reversal symmetry, its dynamic control on ultrafast timescales in nonmagnetic insulating oxides remains virtually unexplored. Here, we demonstrate simultaneous magnetic symmetry lowering and timereversal-symmetry breaking in cubic SrTiO3 driven by an off-resonant, elliptically polarized THz pulse. Second harmonic generation (SHG) polarimetry reveals emergent SHG circular dichroism inconsistent with third-order nonlinear processes under cubic m3m symmetry. The SHG polar patterns exhibit mirror-symmetry breaking, indicating a transient reduction to tetragonal 4/mm'm' magnetic symmetry. Furthermore, the SHG response scales linearly with the angular momentum of THz pulse, providing direct evidence for THz-field-induced timereversal-symmetry breaking. These results establish a direct pathway for ultrafast symmetry control in non-magnetic oxides, enabling dynamic manipulation of emergent phases on ultrafast timescales.

cond-mat.mtrl-sci↗

arXiv2026

Generalizing Thermal Transport in High-Contrast Metamaterials through Interfacial Fresnel Reflection

The rapid growth of generative AI has intensified the need for efficient heat dissipation in large-scale data centers. To control heat flow, thermal metamaterials with layered structures have been widely used, which impart the anisotropic properties of thermal conductivities. However, the conventional effective medium approximation (EMA) often fails to provide accurate predictions in systems with a high thermal conductivity contrast between adjacent layers embedded in a background medium. Here, we generalize the EMA by introducing two corrective coefficients that extend its validity to regimes where the conventional EMA was previously inapplicable, i.e., high-contrast thermal metamaterials with the background medium. Notably, one of these coefficients that we proposed has the same mathematical form as the Fresnel reflection coefficient in optics. This allows us to interpret the "reflection-like" behavior of heat flow as it penetrates adjacent layers with high thermal contrast. Our findings suggest that heat diffusion, traditionally viewed as a purely dissipative process, can be understood intuitively through the framework of ray optics.

physics.optics↗

arXiv2026

Observation of mirror-odd and mirror-even spin texture in ultrathin epitaxially strained RuO2 films

Recently, rutile ruthenium dioxide (RuO$_2$) has attracted renewed interest due to expectations of prominent altermagnetic spin splitting. However, accumulating experimental evidence suggests that, in its bulk and thick-film forms, RuO$_2$ does not display any form of magnetic ordering. Despite this, the spin structure of RuO$_2$ remains largely unexplored in the ultrathin limit, where substrate-imposed epitaxial strain can be substantial. Here, we use spin-resolved angle-resolved photoemission spectroscopy, supported by ab initio calculations, to reveal the electronic structure of 2-nanometer-thick epitaxial RuO$_2$ heterostructures. We observe an unconventional spin texture characterized by the coexistence of mirror-even and mirror-odd momentum-dependent components. A comprehensive symmetry analysis rules out nonmagnetic origins of this spin texture. These findings suggest an emergent nonrelativistic spin structure enabled by epitaxial strain in the ultrathin limit, marking a distinct departure from the behavior of relaxed or bulk RuO$_2$. Our work opens previously unexplored perspectives for exploring symmetry-breaking mechanisms and spin textures in oxide heterostructures.

cond-mat.mtrl-sci↗

arXiv2025

Strain Engineering of van Hove Singularity and Coupled Itinerant Ferromagnetism in Quasi-2D Oxide Superlattices

Engineering van Hove singularities (vHss) near the Fermi level, if feasible, offers a powerful route to control exotic quantum phases in electronic and magnetic behaviors. However, conventional approaches, which rely primarily on chemical and electrical doping, focus mainly on local electrical or optical measurements, limiting their applicability to coupled functionalities. In this study, a vHs-induced insulator-metal transition coupled with a ferromagnetic phase transition was empirically achieved in atomically designed quasi-2D SrRuO3 (SRO) superlattices via epitaxial strain engineering, which has not been observed in conventional 3D SRO systems. Theoretical calculations revealed that epitaxial strain effectively modulates the strength and energy positions of vHs of specific Ru orbitals, driving correlated phase transitions in the electronic and magnetic ground states. X-ray absorption spectroscopy confirmed the anisotropic electronic structure of quasi-2D SRO modulated by epitaxial strain. Magneto-optic Kerr effect and electrical transport measurements demonstrated modulated magnetic and electronic phases. Furthermore, magneto-electrical measurements detected significant anomalous Hall effect signals and ferromagnetic magnetoresistance, indicating the presence of magnetically coupled charge carriers in the 2D metallic regime. This study establishes strain engineering as a promising platform for tuning vHss and resultant itinerant ferromagnetism of low-dimensional correlated quantum systems.

cond-mat.mtrl-sci↗

arXiv2025

Demagnetization-Driven Nanoscale Chirality-Selective Thermal Switch

Chiral-lattice degrees of freedom can offer novel chirality-selective functionalities for thermotronic applications. Chiral phonons, carrying both heat and angular momentum, can emerge through a breaking of chiral degeneracy in the phonon bands, either via an intrinsic chiral crystal structure or by angular momentum transfer from photons or spins. This chiral controllability of the lattice dynamics enables a design of chiral thermo-devices by integrating ferromagnets with chiral materials. Here, we present a nanoscale chirality-selective thermal switch realized using a simple heterostructure composed of ferromagnetic [Co/Pt] multilayers and insulating chiral $α$-SiO2, where an external magnetic field can control thermal transport properties. Our experimental results based on the magneto-optic thermometry reveal that the thermal conductivity of $α$-SiO2 exhibits a clear dependence on both the magnetization direction of [Co/Pt] multilayers and the structural chirality of $α$-SiO2, which is supported well by the first-principles-based molecular dynamic simulations. The magnetization-dependent thermal on/off ratio amounts to 1.07 at room temperature and increases to about 1.2 as temperature decreases to 50 K, due to a reduction of Umklapp phonon-phonon scattering rate in $α$-SiO2. These findings provide the first experimental demonstration of the nanoscale chirality-selective thermal switch based on the ferromagnetic/chiral material heterostructure, highlighting its potential as a key technology for addressing heat dissipation challenges in nanoscale electronic devices.

cond-mat.mtrl-sci↗

arXiv2025

Strain-induced Dynamic Spin-Phonon Coupling in Epitaxial RuO2 Films

Magnetic order parameters in altermagnets can couple to quantized lattice vibration via both piezomagnetic and magnetoelastic effects, leading to the renormalization of phonon dispersion. Here, we demonstrate photo-induced dynamic frequency modulation of THz phonons excited in anisotropically-strained epitaxial RuO2 thin films using ultrafast coherent phonon spectroscopy and time-resolved magneto-optic Kerr effect measurement. A coherent oscillation of a transverse acoustic phonon appears in the sub-THz range with increasing film thickness above 4 nm due to local dislocation arising from the anisotropic strain relaxation, which hosts large non-zero shear strain. Interestingly, this phonon mode exhibits a time-varying mode hardening below ~ 500 K. Furthermore, an optical phonon oscillation emerges in magnetization dynamics of the photo-induced non-equilibrium state, and it becomes significantly softened near the critical temperature, while there is no observable magneto-optic signal in fully-strain-relaxed films. Such notable dynamic frequency modulations in acoustic and optical phonons offer an opportunity to manipulate phonons in the THz range through the spin-phonon coupling controlled by epitaxial design, which can inspire the new class of altermagnetic applications in the ultrafast quantum opto-spintronics.

cond-mat.mtrl-sci↗

arXiv2025

Strain-Stabilized Interfacial Polarization Tunes Work Function Over 1 eV in RuO2/TiO2 Heterostructures

Interfacial polarization-charge accumulation at the heterointerface-is a well-established tool in semiconductors, but its influence in metals remains unexplored. Here, we demonstrate that interfacial polarization can robustly modulate surface work function in metallic rutile RuO2 layers in epitaxial RuO2/TiO2 heterostructures grown by hybrid molecular beam epitaxy. Using multislice electron ptychography, we directly visualize polar displacements of transition metal ions relative to oxygen octahedra near the interface, despite the conductive nature of RuO2. This interfacial polarization enables over 1 eV modulation of the RuO2 work function, controlled by small thickness variation (2-4 nm) as measured by Kelvin probe probe microscopy, with a critical thickness of 4 nm - corresponding to the transition from fully strained to relaxed film. These results establish interfacial polarization as a powerful route to control electronic properties in metals and have implications for designing tunable electronic, catalytic, and quantum devices through interfacial control in polar metallic systems.

cond-mat.mtrl-sci↗

arXiv2025

Altermagnetic Polar Metallic phase in Ultra-Thin Epitaxially-Strained RuO2 Films

Altermagnetism refers to a wide class of magnetic orders featuring magnetic sublattices with opposite spins related by rotational symmetries, resulting in non-trivial spin splitting and magnetic multipoles. However, the direct observation of the altermagnetic order parameter remains elusive. Here, by combining theoretical analysis, electrical transport, X-ray and optical spectroscopies, we establish a phase diagram in hybrid molecular beam epitaxy-grown RuO2/TiO2 (110) films, mapping symmetries along with altermagnetic/electronic/structural phase transitions as functions of film thickness and temperature. This features a novel altermagnetic metallic polar phase in epitaxially-strained 2 nm films, extending the concept of multiferroicity to altermagnets. Such a clear signature of a magnetic phase transition at ~500 K is observed exclusively in ultrathin strained films, unlike in bulk RuO2 single crystals. These results demonstrate the potential of epitaxial heterostructure design to induce altermagnetism, paving the way for emergent novel phases with multifunctional properties.

cond-mat.mtrl-sci↗

arXiv2025

Metallicity and Anomalous Hall Effect in Epitaxially-Strained, Atomically-thin RuO2 Films

The anomalous Hall effect (AHE), a hallmark of time-reversal symmetry breaking, has been reported in rutile RuO2, a debated metallic altermagnetic candidate. Previously, AHE in RuO2 was observed only in strain-relaxed thick films under extremely high magnetic fields (~50 T). Yet, in ultrathin strained films with distinctive anisotropic electronic structures, there are no reports, likely due to disorder and defects suppressing metallicity thus hindering its detection. Here, we demonstrate that ultrathin, fully-strained 2 nm TiO2/t nm RuO2/TiO2 (110) heterostructures, grown by hybrid molecular beam epitaxy, retain metallicity and exhibit a sizeable AHE at a significantly lower magnetic field (< 9 T). Density functional theory calculations reveal that epitaxial strain stabilizes a non-compensated magnetic ground state and reconfigures magnetic ordering in RuO2 (110) thin films. These findings establish ultrathin RuO2 as a platform for strain-engineered magnetism and underscore the transformative potential of epitaxial design in advancing spintronic technologies.

cond-mat.mtrl-sci↗

arXiv2021

Possible persistence of multiferroic order down to bilayer limit of van der Waals material NiI$_{2}$

Realizing a state of matter in two dimensions has repeatedly proven a novel route of discovering new physical phenomena. Van der Waals (vdW) materials have been at the center of these now extensive research activities. They offer a natural way of producing a monolayer of matter simply by mechanical exfoliation. This work demonstrates that the possible multiferroic state with coexisting antiferromagnetic and ferroelectric orders possibly persists down to the bilayer flake of NiI$_{2}$. By exploiting the optical second-harmonic generation technique, both magnitude and direction of the ferroelectric order, arising from the cycloidal spin order, are successfully traced. The possible multiferroic state's transition temperature decreases from 58 K for the bulk to about 20 K for the bilayer. Our observation will spur extensive efforts to demonstrate multi-functionality in vdW materials, which have been tried mostly by using heterostructures of singly ferroic ones until now.

cond-mat.mtrl-sci↗