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Seo Hyoung Chang

Publications and source records attributed to Seo Hyoung Chang.

17 recordsLinked to original sources

Multistage development of short-range spin correlations and weak magnetic order in the two coupled trillium lattices of K2Fe2(MoO4)(PO4)2

Trillium lattices, where magnetic ions form a chiral network of corner-sharing triangles, offer a three-dimensional magnetic framework that can host fragile classical spin-liquid states. Herein, we report on the magnetization, specific heat, electron spin resonance (ESR), and muon spin relaxation ($μ$SR) of K$_{2}$Fe$_{2}$(MoO$_{4}$)(PO$_{4}$)$_{2}$ single crystals. Magnetization measurements reveal strong antiferromagnetic interactions coexisting with weak magnetic order at $T_{\rm N} = 5.2$~K, as evidenced by a $λ$-like anomaly observed in the magnetic susceptibility, a critical enhancement of the muon spin relaxation rate and the wipeout of the ESR signal as the temperature approaches $T_{\rm N}$. Above $T_{\rm N}$, two distinct developments of short-range spin correlations are identified at $T_{\rm H} = 34$~K and $T_{\rm L} = 10$~K, supported by magnetic specific heat anomalies and the temperature dependence of the ESR linewidth and $g$-factor. Upon cooling below $T_{\rm N}$, an anomaly appears at $T^{*} = 3.2$~K in thermodynamic observables and the muon spin relaxation rate, indicative of spin reorientation driven by residual interactions. Despite the presence of magnetic order, $μ$SR experiments reveal dynamically fluctuating spins persisting even in the ordered state. Moreover, the suppression of $T_{\rm N}$ under applied magnetic fields ($μ_{0}H \geq 2$~T) suggests that K$_{2}$Fe$_{2}$(MoO$_{4}$)(PO$_{4}$)$_{2}$ constitutes a promising candidate for exploring field-induced spin-liquid behavior in three-dimensionally coupled trillium lattices.

cond-mat.str-el

Tuning magnetic, lattice, and transport properties in CoNb3S6 via Fe doping

We present a comprehensive investigation of the effects of Fe doping on the lattice dynamics, magnetic ordering, and magneto-transport properties of the intercalated van der Waals antiferromagnets Co1-xFexNb3S6 (x = 0.1 and 0.3). Temperature- and polarization-dependent Raman scattering measurements reveal a pronounced blue shift of the 180 cm-1 phonon mode with increasing Fe concentration, indicating enhanced sensitivity of lattice vibrations to Fe-induced structural and mass effects. While the temperature evolution of the phonon modes is dominated by conventional anharmonic phonon softening, subtle anomalies observed near the Néel temperature for x = 0.1 point to weak spin-phonon coupling. Electrical transport and magnetic susceptibility data show clear signatures of the antiferromagnetic phase transitions at TN ~ 20.5-23.7 K for x = 0.1 and TN ~ 32.0 K for x = 0.3. Out-of-plane magnetization measurements reveal hysteretic behavior with two field-induced transitions for x =0.1, which evolve into a single hysteresis loop at x =0.3, signaling a subtle reconstruction of the magnetic ground state. Magneto-transport measurements for x = 0.1 further display a butterfly-shaped hysteretic magnetoresistance and a weak topological Hall effect; however, both features are strongly suppressed at x = 0.3. These results illustrate the critical role of Fe-induced magnetic structure reconstruction in fine-tuning topological and magnetic transport phenomena in intercalated van der Waals antiferromagnets.

cond-mat.mtrl-sci

Coexistence of anomalous spin dynamics and weak magnetic order in a chiral trillium lattice K2FeSn(PO4)3

Trillium lattices, where magnetic ions form a three-dimensional chiral network of corner-sharing equilateral triangular motifs, offer a prominent platform to explore exotic quantum states. In this work, we report ground-state properties of the $S$ = 5/2 trillium lattice compound K$_{2}$FeSn(PO$_{4}$)$_{3}$ through thermodynamic, electron spin resonance (ESR), and muon spin relaxation ($μ$SR) experiments. Thermodynamic and ESR measurements reveal the two-step evolution of magnetic correlations across $T^{*}$ = 11 K, which results from an interplay between dominant antiferromagnetic Heisenberg interactions and subleading interactions. Below $T^{*}$, \textit{dc} and \textit{ac} magnetic susceptibilities indicate weak \textcolor{black}{magnetic ordering} at $T_{\rm N} \approx 2$ K under low fields, which is suppressed for $μ_{0}H \geq 2$ T, consistent with a power-law dependence of magnetic specific heat at low temperatures. $μ$SR experiments confirm the dominance of persistent spin dynamics and the absence of conventional spin freezing, supporting the subtle nature of weak magnetic ordering coexisting with spin-liquid-like fluctuations. These findings underscore the potential for realizing a classical spin-liquid ground state with exotic excitations in high-spin trillium lattice systems.

cond-mat.str-el

Epitaxial Sr-doped nickelate perovskite thin films and Ruddlesden-Popper phases grown by magnetron sputtering

Sr-doped nickelate, Nd1-xSrxNiO3 (NSNO), perovskite thin films and Ruddlesden-Popper (RP) phases are actively investigated because of their physical properties, such as the metal-insulator transition and superconductivity. However, achieving epitaxial growth of NSNO perovskite and RP phase films in a sputtering system is challenging compared to pulsed laser deposition and molecular beam epitaxy, due to the difficulty in stabilizing nickel oxidation states and minimizing structural defects. Here, we used an off-axis radio frequency (RF) magnetron sputtering to fabricate epitaxial NSNO perovskite and RP phase thin films on SrTiO3 (001) substrates, systematically controlling the growth temperatures. We investigated the thermal stability of the perovskite phase and the structural and electronic characteristics of the RP phase films. These findings provide valuable insights into the synthesis of nickelate RP phase films using RF magnetron sputtering, paving the way for scalable thin films fabrication technologies.

cond-mat.mtrl-sci

Signatures of Floquet Engineering in the proximal Kitaev Quantum Spin Liquid H$_3$LiIr$_2$O$_6$ by tr-RIXS

We present the first circularly polarized Floquet engineering time-resolved Resonant Inelastic X-ray Scattering (tr-RIXS) experiment in H$_3$LiIr$_2$O$_6$, an iridium-based Kitaev system. Our calculations and experimental results are consistent with the modification of the low energy magnetic excitations in H$_3$LiIr$_2$O$_6$ only during illumination by the laser pulse, consistent with the Floquet engineering of the exchange interactions. However, the penetration length mismatch between the X-ray probe and laser pump and the intrinsic complexity of Kitaev magnets prevented us from unequivocally extracting towards which ground H$_3$LiIr$_2$O$_6$ was driven. We outline possible solutions to these challenges for Floquet stabilization and observation of the Kitaev Quantum Spin Liquid limit by RIXS.

cond-mat.str-el

Electrical conductivity enhancement of epitaxially grown TiN thin films

Titanium nitride (TiN) presents superior electrical conductivity with mechanical and chemical stability and compatibility with the semiconductor fabrication process. Here, we fabricated epitaxial and polycrystalline TiN (111) thin films on MgO (111), sapphire (001), and mica substrates at 640oC and room temperature by using a DC sputtering, respectively. The epitaxial films show less amount of surface oxidation than the polycrystalline ones grown at room temperature. The epitaxial films show drastically reduced resistivity (~30 micro-ohm-cm), much smaller than the polycrystalline films. Temperature-dependent resistivity measurements show a nearly monotonic temperature slope down to low temperature. These results demonstrate that high temperature growth of TiN thin films leads to significant enhancement of electrical conductivity, promising for durable and scalable electrode applications.

cond-mat.mtrl-sci

Atomic arrangement of van der Waals heterostructures using X-ray scattering and crystal truncation rod analysis

Vanadium diselenide (VSe2) has intriguing physical properties such as unexpected ferromagnetism at the two-dimensional limit. However, the experimental results for room temperature ferromagnetism are still controversial and depend on the detailed crystal structure and stoichiometry. Here we introduce crystal truncation rod (CTR) analysis to investigate the atomic arrangement of bilayer VSe2 and bilayer graphene (BLG) hetero-structures grown on a 6H-SiC(0001) substrate. Using non-destructive CTR analysis, we were able to obtain electron density profiles and detailed crystal structure of the VSe2/BLG heterostructures. Specifically, the out-of-plane lattice parameters of each VSe2 layer were modulated by the interface compared to that of the bulk VSe2 1T phase. The atomic arrangement of the VSe2/BLG heterostructure provides deeper understanding and insight for elucidating the magnetic properties of the van der Waals heterostructure.

cond-mat.mtrl-sci

Experimental verification of polar structures in ultrathin BaTiO_{3} layers using resonant x-ray reflectivity

Functional devices with ultrathin ferroelectric layers have been attracted as a promising candidate for next-generation memory and logic device applications. Using the ultrathin ferroelectric layers, particularly approaching the two-dimensional limit, however, it is still challenging to control ferroelectric switching and to observe ferroelectricity by spectroscopic tools. In particular, conventional methods such as electrical measurements and piezoelectric response force microscopy are very limited due to leakage currents and the smallness of the ferroelectric signals. Here, we show that the ferroelectricity of ultrathin SrRuO3/BaTiO3/SrRuO3 heterostructures grown on SrTiO3(100) substrates can be measured using resonant x-ray reflectivity (RXRR). This experimental technique can provide an element-specific electronic depth profile as well as increased sensitivity to Ti off-center displacements at the Ti K pre-edge. The depth-sensitivity of RXRR selectively detects the strong polarization dependence of the Ti pre-edge features of ultrathin BaTiO3 layers while discriminating the contribution of the SrTiO3 substrate. This technique verified that the BaTiO3 layer can be ferroelectric down to the lowest experimental limit of a critical thickness of 2.5 unit cells. Our results can open a novel way to explore ultrathin ferroelectric-based nano-electronic devices.

cond-mat.mtrl-sci

Stable hump-like Hall effect and non-coplanar spin textures in SrRuO$_3$ ultrathin film

We observed a hump-like feature in Hall effects of SrRuO$_3$ ultrathin films, and systematically investigated it with controlling thicknesses, temperatures and magnetic fields. The hump-like feature is extremely stable, even surviving as a magnetic field is tilted by as much as 85$^\circ$. Based on the atomic-level structural analysis of a SrRuO$_3$ ultrathin film with a theoretical calculation, we reveal that atomic rumplings at the thin-film surface enhance Dzyaloshinskii-Moriya interaction, which can generate stable chiral spin textures and a hump-like Hall effect. Moreover, temperature dependent resonant X-ray measurements at Ru L-edge under a magnetic field showed that the intensity modulation of unexpected peaks was correlated with the hump region in the Hall effect. We verify that the two-dimensional property of ultrathin films generates stable non-coplanar spin textures having a magnetic order in a ferromagnetic oxide material.

cond-mat.str-el

Modulating Curie Temperature and Magnetic Anisotropy in Nanoscale Layered Cr_{2}Te_{3} Films: Implications for Room-Temperature Spintronics

Nanoscale layered ferromagnets have demonstrated fascinating two-dimensional magnetism down to atomic layers, providing a peculiar playground of spin orders for investigating fundamental physics and spintronic applications. However, strategy for growing films with designed magnetic properties is not well established yet. Herein, we present a versatile method to control the Curie temperature (T_{C}) and magnetic anisotropy during growth of ultrathin Cr_{2}Te_{3} films. We demonstrate increase of the TC from 165 K to 310 K in sync with magnetic anisotropy switching from an out-of-plane orientation to an in-plane one, respectively, via controlling the Te source flux during film growth, leading to different c-lattice parameters while preserving the stoichiometries and thicknesses of the films. We attributed this modulation of magnetic anisotropy to the switching of the orbital magnetic moment, using X-ray magnetic circular dichroism analysis. We also inferred that different c-lattice constants might be responsible for the magnetic anisotropy change, supported by theoretical calculations. These findings emphasize the potential of ultrathin Cr_{2}Te_{3} films as candidates for developing room-temperature spintronics applications and similar growth strategies could be applicable to fabricate other nanoscale layered magnetic compounds.

cond-mat.mtrl-sci

Novel $J_{\rm{eff}}$=3/2 Metallic Phase and Unconventional Superconductivity in GaTa$_4$Se$_8$

By means of density functional theory plus dynamical mean-field theory (DFT+DMFT) calculations and resonant inelastic x-ray scattering (RIXS) experiments, we investigate the high-pressure phases of the spin-orbit-coupled $J_{\rm{eff}}=3/2$ insulator GaTa$_4$Se$_8$. Its metallic phase, derived from the Mott state by applying pressure, is found to carry $J_{\rm{eff}}=3/2$ moments. The characteristic excitation peak in the RIXS spectrum maintains its destructive quantum interference of $J_{\rm{eff}}$ at the Ta $L_2$-edge up to 10.4 GPa. Our exact diagonalization based DFT+DMFT calculations including spin-orbit coupling also reveal that the $J_{\rm{eff}}=3/2$ character can be clearly identified under high pressure. These results establish the intriguing nature of the correlated metallic magnetic phase, which represents the first confirmed example of $J_{\rm{eff}}$=3/2 moments residing in a metal. They also indicate that the pressure-induced superconductivity is likely unconventional and influenced by these $J_{\rm{eff}}=3/2$ moments. Based on a self-energy analysis, we furthermore propose the possibility of doping-induced superconductivity related to a spin-freezing crossover.

cond-mat.str-el

Hump-like structure in Hall signal from SrRuO$_3$ ultra-thin films without inhomogeneous anomalous Hall effect

A controversy arose over the interpretation of the recently observed hump features in Hall resistivity $ρ_{xy}$ from ultra-thin SrRuO$_3$ (SRO) film; it was initially interpreted to be due to topological Hall effect but was later proposed to be from existence of regions with different anomalous Hall effect (AHE). In order to settle down the issue, we performed Hall effect as well as magneto-optic Kerr-effect measurements on 4 unit cell SRO films grown on SrTiO$_3$ (001) substrates. Clear hump features are observed in the measured $ρ_{xy}$, whereas neither hump feature nor double hysteresis loop is seen in the Kerr rotation which should be proportional to the magnetization. In addition, magnetization measurement by superconducting quantum interference device shows no sign of multiple coercive fields. These results show that inhomogeneous AHE alone cannot explain the observed hump behavior in $ρ_{xy}$ data from our SRO ultra-thin films. We found that emergence of the hump structure in $ρ_{xy}$ is closely related to the growth condition, high quality films having clear sign of humps.

cond-mat.str-el

Direct experimental observation of the molecular Jeff=3/2 ground state in the lacunar spinel GaTa4Se8

Strong spin-orbit coupling lifts the degeneracy of t2g orbitals in 5d transition-metal systems, leaving a Kramers doublet and quartet with effective angular momentum of Jeff = 1/2 and 3/2, respectively. These spin-orbit entangled states can host exotic quantum phases such as topological Mott state, unconventional superconductivity, and quantum spin liquid. The lacunar spinel GaTa4Se8 was theoretically predicted to form the molecular Jeff = 3/2 ground state. Experimental verification of its existence is an important first step to exploring the consequences of the Jeff = 3/2 state. Here, we report direct experimental evidence of the Jeff = 3/2 state in GaTa4Se8 by means of excitation spectra of resonant inelastic x-rays scattering at the Ta L3 and L2 edges. We found that the excitations involving the Jeff = 1/2 molecular orbital were suppressed only at the Ta L2 edge, manifesting the realization of the molecular Jeff = 3/2 ground state in GaTa4Se8.

cond-mat.str-el

Oxygen Partial Pressure during Pulsed Laser Deposition: Deterministic Role on Thermodynamic Stability of Atomic Termination Sequence at SrRuO3/BaTiO3 Interface

With recent trends on miniaturizing oxide-based devices, the need for atomic-scale control of surface/interface structures by pulsed laser deposition (PLD) has increased. In particular, realizing uniform atomic termination at the surface/interface is highly desirable. However, a lack of understanding on the surface formation mechanism in PLD has limited a deliberate control of surface/interface atomic stacking sequences. Here, taking the prototypical SrRuO3/BaTiO3/SrRuO3 (SRO/BTO/SRO) heterostructure as a model system, we investigated the formation of different interfacial termination sequences (BaO-RuO2 or TiO2-SrO) with oxygen partial pressure (PO2) during PLD. We found that a uniform SrO-TiO2 termination sequence at the SRO/BTO interface can be achieved by lowering the PO2 to 5 mTorr, regardless of the total background gas pressure (Ptotal), growth mode, or growth rate. Our results indicate that the thermodynamic stability of the BTO surface at the low-energy kinetics stage of PLD can play an important role in surface/interface termination formation. This work paves the way for realizing termination engineering in functional oxide heterostructures.

cond-mat.mtrl-sci

Enhanced electrocatalytic activity via phase transitions in strongly correlated SrRuO3 thin films

Transition metal oxides have been extensively studied and utilized as efficient catalysts. However, the strongly correlated behavior which often results in intriguing emergent phenomena in these materials has been mostly overlooked in understanding the electrochemical activities. Here, we demonstrate a close correlation between the phase transitions and oxygen evolution reaction (OER) in a strongly correlated SrRuO3. By systematically introducing Ru-O vacancies into the single-crystalline SrRuO3 epitaxial thin films, we induced phase transition in crystalline symmetry which resulted in corresponding modification in the electronic structure. The modified electronic structure significantly affect the electrochemical activities, so a 30% decrease in the overpotential for the OER activity was achieved. Our study suggests that a substantial enhancement in the OER activity can be realized even within single material systems, by rational design and engineering of their crystal and electronic structures.

cond-mat.str-el

Interface control of ferroelectricity in a SrRuO3/BaTiO3/SrRuO3 capacitor and its critical thickness

The atomic-scale synthesis of artificial oxide heterostructures offers new opportunities to create novel states that do not occur in nature. The main challenge related to synthesizing these structures is obtaining atomically sharp interfaces with designed termination sequences. Here, we demonstrate that the oxygen pressure (PO2) during growth plays an important role in controlling the interfacial terminations of SrRuO3/BaTiO3/SrRuO3 (SRO/BTO/SRO) ferroelectric capacitors. The SRO/BTO/SRO heterostructures were grown by the pulsed laser deposition (PLD) method. The top SRO/BTO interface grown at high PO2 (around 150 mTorr) usually exhibited a mixture of RuO2-BaO and SrO-TiO2 terminations. By reducing PO2, we obtained atomically sharp SRO/BTO top interfaces with uniform SrO-TiO2 termination. Using capacitor devices with symmetric and uniform interfacial termination, we were able to demonstrate for the first time that the ferroelectric (FE) critical thickness can reach the theoretical limit of 3.5 unit cells (u.c.).

cond-mat.mtrl-sci

Temperature Evolution of Itinerant Ferromagnetism in SrRuO3 Probed by Optical Spectroscopy

The temperature ($T$) dependence of the optical conductivity spectra $σ(ω)$ of a single crystal SrRuO$_3$ thin film is studied over a $T$ range from 5 to 450 K. We observed significant $T$ dependence of the spectral weights of the charge transfer and interband $d$-$d$ transitions across the ferromagnetic Curie temperature ($T_c$ ~ 150 K). Such $T$ dependence was attributed to the increase in the Ru spin moment, which is consistent with the results of density functional theory calculations. $T$ scans of $σ(Ω, T)$ at fixed frequencies $Ω$ reveal a clear $T^2$ dependence below $T_c$, demonstrating that the Stoner mechanism is involved in the evolution of the electronic structure. In addition, $σ(Ω, T)$ continues to evolve at temperatures above $T_c$, indicating that the local spin moment persists in the paramagnetic state. This suggests that SrRuO$_3$ is an intriguing oxide system with itinerant ferromagnetism.

cond-mat.str-el