arXiv subjects

Jeong Rae Kim

Publications and source records attributed to Jeong Rae Kim.

15 recordsLinked to original sources

arXiv2026

AlV$_2$O$_4$ thin films via in-situ interfacial topotaxy

Conventional oxide epitaxy approaches face challenges when the oxidation conditions of constituent elements differ significantly. Here we demonstrate that V--O thin films can serve as solid-phase precursors for epitaxial AlV$_2$O$_4$, comprising a pyrochlore V$^{2.5+}$ network coexisting with AlO$_4$ tetrahedra within the spinel structure. The epitaxial AlV$_2$O$_4$/Al$_2$O$_3$ (0001) heterostructures are realized via interfacial topotactic transformation, involving V--O growth at a moderate temperature followed by in-situ ultra-high-temperature post-annealing to drive a reaction with the Al$_2$O$_3$ substrate. Transmission electron microscopy and temperature-dependent X-ray diffraction analyses reveal excellent structural characteristics that closely reproduce the known charge-ordering transition. This study presents a novel approach to realizing epitaxial structures with convoluted oxidation states where thermodynamic and kinetic barriers would otherwise limit synthesizability.

cond-mat.mtrl-sci↗

arXiv2026

Identification of the I$_{10}$ Donor in ZnO as a Sn--Li Complex with Large Hyperfine Interaction

Donor impurities in wide direct band gap semiconductors provide a promising platform for spin--photon quantum technologies by combining a donor spin qubit with optically addressable transitions. In ZnO, the shallow donor with the largest reported binding energy has long been associated with the I$_{10}$ bound exciton line, but its microscopic origin has remained unresolved. Here we demonstrate the controlled formation and identification of this donor as a Sn--Li complex through a combination of ion implantation, annealing, optical spectroscopy, and first-principles calculations. Resonant two-laser coherent population trapping measurements reveal an electron--$^{119}$Sn hyperfine interaction of $392 \pm 15$\,MHz, establishing a coupled electron--spin--1/2, nuclear--spin--1/2 system with one of the largest hyperfine couplings reported for shallow donors in semiconductors. Density functional theory calculations show that a nearest-neighbor Sn$_{\mathrm{Zn}}$--Li$_{\mathrm{Zn}}$ complex has favorable formation energetics, donor character with the electron localized on Sn, and an extrapolated hyperfine interaction consistent with experiment. The large donor binding energy and excited-state structure indicate enhanced thermal robustness of the optical transition relative to conventional group--III donors, while the strong hyperfine interaction enables fast electron--nuclear spin control and prospects for direct nuclear--spin--photon interfaces. We further observe efficient optically induced nuclear spin polarization, highlighting a path toward nuclear spin initialization. More broadly, our results reveal how a donor--acceptor complex can access previously unexplored regimes of shallow donor physics, extending the design space of quantum defects beyond isolated substitutional dopants.

quant-ph↗

arXiv2026

Thermally-Activated Epitaxy of NbO

We demonstrate a thermally-activated epitaxy window for the growth of NbO at temperatures exceeding 1000 $^o$C. NbO films grown in this mode display superior structural and transport properties, which are reproducible across a window of oxygen partial pressure. Through comprehensive analysis, we propose the prototypical electrical properties of NbO, for which a consensus has not yet been made. This study unequivocally demonstrates the utility of high temperatures in the thin film synthesis of refractory metal compounds.

cond-mat.mtrl-sci↗

arXiv2025

Superconducting vacancy-ordered rock-salt NbO films

We report molecular beam epitaxy synthesis of vacancy-ordered rocksalt NbO thin films which display superconductivity. A comparative study of substrates identifies Al$_2$O$_3$ (0001) as the optimal platform for realizing high-quality, single-phase films when growing at temperatures exceeding 1000 $^\circ$C. The controlled NbO films exhibit superconductivity with critical temperatures up to $T_\mathrm{c}$ = 1.37 K, comparable to bulk single crystals. This work addresses the fundamental bottlenecks encountered in the high-temperature epitaxy of compounds with uncommon oxidation states, while expanding the scope of available thin-film superconductors.

cond-mat.supr-con↗

arXiv2024

High temperature diffusion enabled epitaxy of the Ti-O system

High temperatures promote kinetic processes which can drive crystal synthesis towards ideal thermodynamic conditions, thereby realizing samples of superior quality. While accessing very high temperatures in thin-film epitaxy is becoming increasingly accessible through laser-based heating methods, demonstrations of such utility are still emerging. Here we realize a novel self-regulated growth mode in the Ti-O system by relying on thermally activated diffusion of oxygen from an oxide substrate. We demonstrate oxidation selectivity of single phase films with superior crystallinity to conventional approaches as evidenced by structural and electronic measurements. The diffusion-enabled mode is potentially of wide use in the growth of transition metal oxides, opening up new opportunities for ultra-high purity epitaxial platforms based on d -orbital systems.

cond-mat.mtrl-sci↗

arXiv2022

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↗

arXiv2022

Heteroepitaxial control of Fermi liquid, Hund metal, and Mott insulator phases in the single-atomic-layer limit

Interfaces between dissimilar correlated oxides can offer devices with versatile functionalities. In that respect, manipulating and measuring novel physical properties of oxide heterointerfaces are highly desired. Yet, despite extensive studies, obtaining direct information on their momentum-resolved electronic structure remains a great challenge. This is because most correlated interfacial phenomena appear within a few atomic layers from the interface, thus limiting the application of available experimental probes. Here, we utilize atomic-scale epitaxy and photoemission spectroscopy to demonstrate the interface control of correlated electronic phases in atomic-scale ruthenate--titanate heterostructures. While bulk SrRuO$_3$ is a ferromagnetic metal, the heterointerfaces exclusively realize three distinct correlated phases in the single-atomic-layer limit. Our theory reveals that atomic-scale structural proximity effects lead to the emergence of Fermi liquid, Hund metal, and Mott insulator phases in the quantum-confined SrRuO$_3$. These results highlight the extensive interfacial tunability of electronic phases, hitherto hidden in the atomically thin correlated heterostructure.

cond-mat.str-el↗

arXiv2021

Observation of spin-dependent dual ferromagnetism in perovskite ruthenates

We performed in-situ angle-resolved photoemission spectroscopy (ARPES) and spin-resolved ARPES (SARPES) experiments to investigate the relationship between electronic band structures and ferromagnetism in SrRuO$_3$ (SRO) thin films. Our high-quality ARPES and SARPES results show clear spin-lifted band structures. The spin polarization is strongly dependent on momentum around the Fermi level, whereas it becomes less dependent at high-binding energies. This experimental observation matches our dynamical mean-field theory (DMFT) results very well. As temperature increases from low to the Curie temperature, spin-splitting gap decreases and band dispersions become incoherent. Based on the ARPES study and theoretical calculation results, we found that SRO possesses spin-dependent electron correlations in which majority and minority spins are localized and itinerant, respectively. Our finding explains how ferromagnetism and electronic structure are connected, which has been under debate for decades in SRO.

cond-mat.str-el↗

arXiv2021

Observation of metallic electronic structure in a single-atomic-layer oxide

Correlated electrons in transition metal oxides (TMOs) exhibit a variety of emergent phases. When TMOs are confined to a single-atomic-layer thickness, experiments so far have shown that they usually lose diverse properties and become insulators. In an attempt to extend the range of electronic phases of the single-atomic-layer oxide, we search for a metallic phase in a monolayer-thick epitaxial SrRuO$_3$ film. Combining atomic-scale epitaxy and angle-resolved photoemission measurements, we show that the monolayer SrRuO$_3$ is a strongly correlated metal. Systematic investigation reveals that the interplay between dimensionality and electronic correlation makes the monolayer SrRuO$_3$ an incoherent metal with orbital-selective correlation. Furthermore, the unique electronic phase of the monolayer SrRuO$_3$ is found to be highly tunable, as charge modulation demonstrates an incoherent-to-coherent crossover of the two-dimensional metal. Our work emphasizes the potentially rich phases of single-atomic-layer oxides and provides a guide to the manipulation of their two-dimensional correlated electron systems.

cond-mat.str-el↗

arXiv2021

Growth and atomically resolved polarization mapping of ferroelectric $Bi_2WO_6$ thin film

Aurivillius ferroelectric $Bi_2WO_6$ (BWO) encompasses a broad range of functionalities, including robust fatigue-free ferroelectricity, high photocatalytic activity, and ionic conductivity. Despite these promising characteristics, an in-depth study on the growth of BWO thin films and ferroelectric characterization, especially at the atomic scale, is still lacking. Here, we report pulsed laser deposition (PLD) of BWO thin films on (001) $SrTiO_3$ substrates and characterization of ferroelectricity using the scanning transmission electron microscopy (STEM) and piezoresponse force microscopy (PFM) techniques. We show that the background oxygen gas pressure used during PLD growth mainly determines the phase stability of BWO films, whereas the influence of growth temperature is comparatively minor. Atomically resolved STEM study of a fully strained BWO film revealed collective in-plane polar off-centering displacement of W atoms. We estimated the spontaneous polarization value based on polar displacement mapping to be about 54 $\pm$ 4 $μC cm^{-2}$, which is in good agreement with the bulk polarization value. Furthermore, we found that pristine film is composed of type-I and type-II domains, with mutually orthogonal polar axes. Complementary PFM measurements further elucidated that the coexisting type-I and type-II domains formed a multidomain state that consisted of 90$°$ domain walls (DWs) alongside multiple head-to-head and tail-to-tail 180$°$ DWs. Application of an electrical bias led to in-plane 180$°$ polarization switching and 90$°$ polarization rotation, highlighting a unique aspect of domain switching, which is immune to substrate-induced strain.

cond-mat.mtrl-sci↗

arXiv2021

Electronic band structure of (111) $SrRuO_{3}$ thin film$-$an angle-resolved photoemission spectroscopy study

We studied the electronic band structure of pulsed laser deposition (PLD) grown (111)-oriented SrRuO$_3$ (SRO) thin films using \textit{in situ} angle-resolved photoemission spectroscopy (ARPES) technique. We observed previously unreported, light bands with a renormalized quasiparticle effective mass of about 0.8$m_{e}$. The electron-phonon coupling underlying this mass renormalization yields a characteristic "kink" in the band dispersion. The self-energy analysis using the Einstein model suggests five optical phonon modes covering an energy range 44 to 90 meV contribute to the coupling. Besides, we show that the quasiparticle spectral intensity at the Fermi level is considerably suppressed, and two prominent peaks appear in the valance band spectrum at binding energies of 0.8 eV and 1.4 eV, respectively. We discuss the possible implications of these observations. Overall, our work demonstrates that high-quality thin films of oxides with large spin-orbit coupling can be grown along the polar (111) orientation by the PLD technique, enabling \textit{in situ} electronic band structure study. This could allow for characterizing the thickness-dependent evolution of band structure of (111) heterostructures$-$a prerequisite for exploring possible topological quantum states in the bilayer limit.

cond-mat.str-el↗

arXiv2017

Electronic Reconstruction Enhanced Tunneling Conductance at Terrace Edges of Ultrathin Oxide Films

Quantum mechanical tunneling of electrons across ultrathin insulating oxide barriers has been studied extensively for decades due to its great potential in electronic device applications. In the few-nanometer-thick epitaxial oxide films, atomic-scale structural imperfections, such as the ubiquitously existed one-unit-cell-high terrace edges, can dramatically affect the tunneling probability and device performance. However, the underlying physics has not been investigated adequately. Here, taking ultrathin BaTiO3 films as a model system, we report an intrinsic tunneling conductance enhancement near the terrace edges. Scanning probe microscopy results demonstrate the existence of highly-conductive regions (tens of nanometers-wide) near the terrace edges. First-principles calculations suggest that the terrace edge geometry can trigger an electronic reconstruction, which reduces the effective tunneling barrier width locally. Furthermore, such tunneling conductance enhancement can be discovered in other transition-metal-oxides and controlled by surface termination engineering. The controllable electronic reconstruction could facilitate the implementation of oxide electronic devices and discovery of exotic low-dimensional quantum phases.

cond-mat.mtrl-sci↗

arXiv2017

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↗

arXiv2017

Overcoming the Fundamental Barrier Thickness Limits of Ferroelectric Tunnel Junctions through BaTiO3/SrTiO3 Composite Barriers

Ferroelectric tunnel junctions (FTJs) have attracted increasing research interest as a promising candidate for non-volatile memories. Recently, significant enhancements of tunneling electroresistance (TER) have been realized through modifications of electrode materials. However, direct control of the FTJ performance through modifying the tunneling barrier has not been adequately explored. Here, adding a new direction to FTJ research, we fabricated FTJs with BaTiO3 single barriers (SB-FTJs) and BaTiO3/SrTiO3 composite barriers (CB-FTJs), and reported a systematic study of FTJ performances by varying the barrier thicknesses and compositions. For the SB-FTJs, the TER is limited by pronounced leakage current for ultrathin barriers and extremely small tunneling current for thick barriers. For the CB-FTJs, the extra SrTiO3 barrier provides an additional degree of freedom to modulate the barrier potential and tunneling behavior. The resultant high tunability can be utilized to overcome the barrier thickness limits and enhance the overall CB-FTJ performances beyond those of SB-FTJ. Our results reveal a new paradigm to manipulate the FTJs through designing multilayer tunneling barriers with hybrid functionalities.

cond-mat.mtrl-sci↗

arXiv2017

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↗