arXiv subjects

Seung Gyo Jeong

Publications and source records attributed to Seung Gyo Jeong.

At least 19 recordsLinked to original sources

arXiv2026

Giant Magnetization Enhancement at Ultrathin Limit of an Orthoferrite

Low-dimensional magnetic systems have received significant interest due to their high scalability and energy efficiency for future electromagnetic applications. However, low-dimensional magnetism at finite temperature is subject to Mermin-Wagner fluctuations, which make its realization highly challenging. Here, we propose structural modulation in the thin-film structure of an orthoferrite system to achieve a high low-dimensional magnetic response at room temperature. ErFeO3 epitaxial thin film with atomically precise thickness control demonstrates that the magnetic response at 300 K can be significantly enhanced compared to its bulk counterpart. The magnetic response reaches its maximum value of 3.7 MuB/f.u. for the 2 nm-thick epitaxial film. The characteristic domain structure resulting from epitaxial strain and orbital reconstruction at the surface, both arising from the thin film geometry, has been proposed as the microscopic origin of the giant magnetization enhancement. We show that magnetic ordering can indeed be realized in the 2D limit, with deliberate structural control of orthoferrite systems.

cond-mat.mtrl-sci↗

arXiv2026

Quasicrystalline oxide interfaces by twisting SrTiO3 membranes

Quasicrystals reveal that long-range order can exist without translational periodicity, but deterministic routes for designing strongly bonded quasicrystalline interfaces remain unexplored. Here, we show that such interfaces can be engineered by growing epitaxial SrTiO3 membranes on a sacrificial layer, releasing them, twisting them by prescribed angles, and bonding them onto a chosen substrate. SrTiO3 bilayers twisted by 45° form an octagonal quasicrystalline interface with eight-fold rotational symmetry, whereas trilayers assembled with successive 30° rotations form a dodecagonal interface with twelve-fold symmetry. Selected-area and nano-beam electron diffraction, multislice electron ptychography, atomic-resolution dark field imaging, Fourier analysis, and real-space tiling establish long-range quasicrystalline order with electronic reconstruction evident from electron energy-loss spectroscopy after annealing. Atomistic simulations based on machine-learned interatomic potentials show that octagonal order emerges as the bilayer twist angle approaches 45°. Polarization-dependent X-ray absorption spectroscopy in 1.5 nm twisted bilayers reveals a twist-dependent electronic response, and terahertz-field-induced second-harmonic generation circular dichroism identifies a symmetry-dependent nonlinear optical response at the 45° quasicrystalline condition. Twisted oxide membranes therefore provide an extendable route to engineer quasiperiodic order and couple it to interfacial bonding, orbital reconstruction, and nonlinear optical response in complex oxides.

cond-mat.mtrl-sci↗

arXiv2026

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↗

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

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↗

arXiv2026

Epitaxial Strain Activates Altermagnetic Spin-Splitting Torques in RuO2(100)

The altermagnetic nature of rutile RuO2 remains under active debate: bulk measurements indicate a nearly nonmagnetic ground state, whereas thin-film studies have reported symmetry-dependent transport signatures consistent with altermagnetism. Here, we provide experimental evidence that altermagnetic spin splitting in RuO2 is a strain-stabilized emergent state rather than an intrinsic bulk property. Angular-resolved spin-torque measurements reveal a symmetry-selected spin Hall response characteristic of altermagnetic spin splitting, which is strongest in the strained regime but progressively suppressed as the lattice relaxes toward the bulk limit. Complementary magnetic measurements further reveal enhanced coercivity and exchange-bias behavior exclusively in strained films, indicating the emergence of a strain-stabilized magnetic state. First-principles calculations reproduce the strain-dependent evolution of the Neel order and spin-split electronic structure, supporting the experimental observations. Together, these results establish altermagnetic spin splitting in RuO2 as a strain-stabilized emergent state and provide a unified explanation for the long-standing discrepancy between bulk and thin-film observations.

cond-mat.mtrl-sci↗

arXiv2026

Strain-Driven Altermagnetic Spin Splitting Effect in RuO$_2$

The non-relativistic spin-momentum locking in altermagnets gives rise to a time-reversal-odd spin Hall effect, known as the altermagnetic spin-splitting effect (ASSE). Although ASSE was first reported in RuO$_2$, subsequent experiments have yielded inconsistent results, leaving its spin-transport mechanism unclear. Here, we systematically investigate how strain, crystal orientation, and the Hubbard $U$ parameter influence the magnetic ground state and spin Hall response of RuO$_2$. Guided by recent experimental observations, we find that $U$ is likely smaller than the value required to induce intrinsic magnetism, suggesting that bulk RuO$_2$ and (001)/(101) RuO$_2$ thin films grown on TiO$_2$ are nonmagnetic in the absence of extrinsic effects. In contrast, (100) and (110) films exhibit strain-induced altermagnetic spin splitting, leading to a strong ASSE even without Hubbard $U$ corrections. These results reconcile previous experimental discrepancies and provide design guidelines for RuO$_2$-based spintronic devices.

cond-mat.mtrl-sci↗

arXiv2026

Magneto-Optical Detection of Anisotropic Spin Currents in Altermagnetic RuO2

Altermagnets are a recently identified class of collinear antiferromagnets that host large spin-split electronic bands, offering a promising platform for efficient spin-current generation. Among proposed candidates, the metallic oxide RuO2 is predicted to exhibit strong altermagnetic spin splitting; however, whether it sustains robust magnetic order beyond the ultrathin thickness limit remains unresolved. Here, we employ optical probes to investigate charge-to-spin conversion in a 12-nm-thick (101)-oriented RuO2 film grown on sapphire. Polarization-resolved second-harmonic generation reveals nonlinear optical responses consistent with the surface symmetry and Néel order of RuO2. Under an applied current, both second-harmonic generation and polar magneto-optical Kerr effect measurements detect a pronounced, directionally anisotropic spin polarization, exhibiting enhanced signals for current along [010] and strongly suppressed responses for current along [-101], in agreement with the symmetry of the altermagnetic spin-splitter effect. Non-magnetic or Rashba-type mechanisms cannot explain this symmetry-selective response. Scanning transmission electron microscopy further reveals that substantial strain persists even in relatively thick films, providing a possible explanation for the observed behavior. Therefore, these results establish RuO2 as an efficient spin source and demonstrate the potential of altermagnets for field-free spintronic devices.

cond-mat.mtrl-sci↗

arXiv2026

Strain Engineering of Altermagnetic Symmetry in Epitaxial RuO$_2$ Films

The magnetic ground state of RuO$_2$ has been under intense debate. Using first-principles calculations, we show that compressive strain along [001] direction stabilizes an altermagnetic phase in RuO$_2$ thin films grown on (100) and (110) TiO$_2$ substrates. We further identify that compressive strain enhances the density of states near the Fermi level, resulting in a Fermi surface instability and the emergence of altermagnetism. The magnitude of strain and the associated increase in the density of states can be tuned by varying the film thickness, as systematically confirmed by x-ray diffraction and photoemission spectroscopy measurements. Symmetry analysis further reveals that (100) RuO$_2$ hosts an ideal altermagnetic order, whereas broken symmetry in (110) films leads to an uncompensated ferrimagnetic state. Finally, we discuss the effects of Hubbard $U$ parameters and evaluate the realistic tunneling magnetoresistance of (100) RuO$_2$.

cond-mat.mtrl-sci↗

arXiv2026

Emergence of unconventional magnetic order in strain-engineered RuO2/TiO2 superlattices

The spin ordering in RuO2 remains a highly debated topic, owing to its elusive nature, with reports ranging from a nonmagnetic ground state to signatures of unconventional magnetic order. Here we provide the first unambiguous, and direct evidence of unconventional magnetism in epitaxial, fully strained RuO2/TiO2 superlattices on TiO2 (110) substrate grown by hybrid molecular beam epitaxy. Polarized neutron reflectometry reveals a finite magnetic moment localized within the compressively strained RuO2 layers, consistent with predictions obtained from first-principles calculations. Complementary density functional theory and X-ray photoemission spectroscopy show that epitaxial strain drives the Ru 4d states toward the Fermi level, triggering a Stoner-type instability that stabilizes non-compensated magnetic order. These unique results reveal that RuO2 exhibits unconventional magnetic states under epitaxial strain, which are not accessible in bulk and establish strain engineering as a powerful route to uncover and control magnetic phases in RuO2 and related oxides.

cond-mat.mtrl-sci↗

arXiv2026

Wafer-scale High-k SrTiO3 Dielectrics with Rational Barrier-layer Design for Low Leakage and High Charge Density

High-k oxides such as SrTiO3 promise large capacitance, but their dielectric response is often limited by leakage currents due to reduced bandgaps. We show that introducing a thin barrier layer beneath SrTiO3 is a simple and effective way to suppress leakage and increase charge density. Using hybrid molecular beam epitaxy, we grew uniform SrTiO3 films on Nb:SrTiO3, CaSnO3/Nb:SrTiO3, and 2-inch SiO2/p-Si stacks to directly compare how different barrier layers influence device behavior. Both CaSnO3 and SiO2 reduce leakage, but the ultra-wide-bandgap SiO2 layer enables much higher operating voltages, yielding charge densities exceeding 5x10^13 cm^-2 at room temperature - more than a fivefold enhancement compared to devices without a barrier layer. This improvement comes with a predictable trade-off: the lower dielectric constant of SiO2 reduces overall capacitance, making its thickness an important design parameter. Together, these results demonstrate that rational barrier-layer engineering - including wafer-scale integration on Si - provides a clear pathway to achieving higher charge densities in SrTiO3-based dielectric devices.

cond-mat.mtrl-sci↗

arXiv2025

Awakening catalytically active surface of BaRuO3 thin film for alkaline hydrogen evolution

The dynamic reconstruction of surfaces during electrochemical reactions plays a crucial role in determining the performance of electrocatalysts. However, because reconstructions occur at the atomic level, direct observation and elucidation of the underlying mechanism are challenging for conventional powder type catalysts with ill defined lattices. In this study, the catalytically active surface of 3C BaRuO3 (BRO) epitaxial thin films emerges upon the dynamic introduction of surface Ru clusters, for the alkaline hydrogen evolution reaction (HER). Based on the mass activity at overpotential 100 mV, the intrinsic HER performance increases dramatically from 0.11 to 7.72 A/mg immediately after the initial HER cycle and eventually saturates at 1.05 A/mg after continuous operation. The formation of Ru clusters on the catalyst surface, driven by selective Ba leaching under alkaline HER conditions, is observed experimentally. Density functional theory calculations demonstrate that HER activity increased with enhanced H* adsorption owing to the dynamic Ru6 cluster formation. A strategy for stabilizing the 'awakened' active surface of BRO is further proposed by validating that the atomic-scale control of the film thickness can effectively maintain the highly active state. This study offers fundamental insights into the design and stabilization of the highly active Ru-based electrocatalysts for the alkaline HER.

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

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

Coexistence of unconventional spin Hall effect and antisymmetric planar Hall effect in IrO$_2$

Crystal symmetry plays an important role in the Hall effects. Unconventional spin Hall effect (USHE), characterized by Dresselhaus and out-of-plane spins, has been observed in materials with low crystal symmetry. Recently, antisymmetric planar Hall effect (APHE) was discovered in rutile RuO2 and IrO2 (101) thin films, which also exhibit low crystal symmetry. In this study, we report the observation of both USHE and APHE in IrO2 (111) films, using spin-torque ferromagnetic resonance (ST-FMR) and harmonic Hall measurements, respectively. Notably, the unconventional spin torque efficiency from Dresselhaus spin was more than double that of a previous report. Additionally, the temperature dependence of APHE suggests that it arises from the Lorentz force, constrained by crystal symmetry. Symmetry analysis supports the coexistence of USHE and APHE and demonstrates that both originate from the crystal symmetry of IrO2 (111), paving the way for a deeper understanding of Hall effects and related physical phenomena.

cond-mat.mes-hall↗

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↗

arXiv2024

Dimensionality Engineering of Magnetic Anisotropy from Anomalous Hall Effect in Synthetic SrRuO3 Crystals

Magnetic anisotropy in atomically thin correlated heterostructures is essential for exploring quantum magnetic phases for next-generation spintronics. Whereas previous studies have mostly focused on van der Waals systems, here, we investigate the impact of dimensionality of epitaxially-grown correlated oxides down to the monolayer limit on structural, magnetic, and orbital anisotropies. By designing oxide superlattices with a correlated ferromagnetic SrRuO3 and nonmagnetic SrTiO3 layers, we observed modulated ferromagnetic behavior with the change of the SrRuO3 thickness. Especially, for three-unit-cell-thick layers, we observe a significant 1,500% improvement of coercive field in the anomalous Hall effect, which cannot be solely attributed to the dimensional crossover in ferromagnetism. The atomic-scale heterostructures further reveal the systematic modulation of anisotropy for the lattice structure and orbital hybridization, explaining the enhanced magnetic anisotropy. Our findings provide valuable insights into engineering the anisotropic hybridization of synthetic magnetic crystals, offering a tunable spin order for various applications.

cond-mat.mtrl-sci↗