arXiv subjects

Suk Hyun Sung

Publications and source records attributed to Suk Hyun Sung.

At least 19 recordsLinked to original sources

arXiv2026

Nanoscale Polar Landscapes in Quantum Paraelectric SrTiO3

SrTiO3 is a textbook quantum paraelectric, with ferroelectricity purportedly suppressed by quantum fluctuations of ionic positions down to the lowest temperatures. The precise real space structure of SrTiO3 at low temperature, however, has remained undefined despite decades of study. Here we directly image the low-temperature polar structure of quantum parelectric SrTiO3, using cryogenic scanning transmission electron microscopy down to 20 K. High resolution imaging reveals a spatially fluctuating landscape of nanoscale domains of finite polarization. The short-range polar domains first grow and self-organize into a periodic structure over tens of nanometers. However, the process reverses when entering the quantum paraelectric regime below 40 K and the periodically ordered polar nanodomains fragment into small clusters.

cond-mat.mtrl-sci↗

arXiv2026

Melting of Charge Density Waves in Low Dimensions

Charge density waves (CDWs) are collective electronic states that can reshape and melt, even while confined within a rigid atomic crystal. In two dimensions, melting is predicted to be distinct, proceeding through partially ordered nematic and hexatic states that are neither liquid nor crystal. Here we measure and explain how continuous, hexatic melting of incommensurate CDWs occurs in low-dimensional materials. As a CDW is thermally excited, disorder emerges progressively$\unicode{x2013}$initially through smooth elastic deformations that modulate the local wavelength, and subsequently via the nucleation of topological defects. Experimentally, we track three hallmark signatures of CDW melting$\unicode{x2013}$azimuthal superlattice peak broadening, wavevector contraction, and integrated intensity decay.

cond-mat.mtrl-sci↗

arXiv2026

Helium-Cooled Cryogenic STEM Imaging and Ptychography for Atomic-Scale Study of Low-Temperature Phases

Much of the exotic functionality of prime interest in quantum materials emerges from structural and electronic ground states that can only be accessed at cryogenic temperatures. Understanding device operation therefore requires structural characterization under the same low-temperature conditions at which these functional phases exist, as room-temperature measurements often probe a different structural state. Achieving atomic-resolution in scanning transmission electron microscopy imaging and particularly 4D-STEM electron ptychography at liquid helium temperature has remained extremely challenging because even small amounts of drift, vibration, and thermal instability associated with the cryogen can disrupt the stringent stability requirements of atomic-resolution STEM. In this work we demonstrate atomic-resolution STEM and multislice electron ptychography at temperatures as low as 20 K using a commercial helium cooled holder. We find that rapid scans and a multi-stage registration workflow are critical to reducing artifacts associated with cryogenic instability for atomic-resolution imaging, while for ptychography scan position correction including compensation for coupling between probe aberrations and position refinement is necessary for successful reconstructions. Together these results establish a pathway for reliable atomic-resolution STEM and ptychography at low temperature, enabling direct visualization of structural ground states relevant to quantum technology.

cond-mat.mtrl-sci↗

arXiv2026

Kondo driven suppression of charge density wave in Van der Waals material UTe$_3$

Competing electronic instabilities lie at the heart of emergent phenomena in quantum materials. In low-dimensional metals, Fermi-surface nesting can drive charge density wave (CDW) formation through a Peierls-like mechanism, while in strongly correlated systems, Kondo hybridization reconstructs the electronic structure by entangling localized moments with itinerant electrons. How these two fundamentally different instabilities interact$-$whether they coexist, compete, or mutually exclude each other$-$remains an open question. Here, we present suppression of charge density wave via the Kondo interaction in van der Waals material UTe$_3$. The angle-resolved photoemission spectroscopy (ARPES) data reveals Fermi surface nesting under similar conditions as seen in RETe$_3$ compounds. Despite that, no CDW is found in UTe$_3$ after an extensive search. We demonstrate that strong hybridization between U 5$f$ electrons and Te $p$ states reconstructs the low-energy electronic structure, removes the instability, and preempts CDW formation. Our results reveal a rare example where Kondo hybridization preempts density wave formation, offering a new route to controlling ordering phenomena in correlated 2D materials.

cond-mat.str-el↗

arXiv2026

Kondo Reshapes Multiple Orders in a $5f$ van der Waals Material

Electron interactions can drive magnetism, superconductivity, and topology. However, the realization of these phases remains limited in van der Waals materials, and the full landscape of strong correlations remains uncharted in any context. While interactions between conduction electrons and localized spins yield a well-known competition between heavy fermions (Kondo hybridization) and magnetic order (RKKY exchange), such spin-driven competition represents only part of the correlated electron phase diagram. Here we demonstrate that a heavy-fermion state can also compete with charge order, such as the charge density wave (CDW) state typical in the van der Waals $4f$ rare-earth tritellurides (RTe$_3$). We exploit the spatially-extended $5f$ orbitals of $β$-UTe$_3$ to enhance Kondo hybridization compared to its isostructural RTe$_3$ cousins. Our scanning tunneling spectroscopy on $β$-UTe$_3$ shows Fano resonances characteristic of the heavy fermion state, while our quasiparticle interference imaging reveals the disappearance of Fermi-level nesting and the appearance of flat bands. We extend the tritelluride tight-binding model to include Kondo coupling and quantify the Fermi surface reconstruction. Consistent with the destruction of nesting, we observe no CDW in $β$-UTe$_3$. Our expansion of the Kondo phase diagram beyond spin-mediated competition opens new possibilities for proximity-induced phase engineering in correlated van der Waals heterostructures.

cond-mat.str-el↗

arXiv2025

Mesoscopic Helices of Polar Domains in a Quadruple Perovskite

A significant effort in condensed matter physics is dedicated to the search for exotic arrangements of electric dipoles in crystals. Non-collinear dipolar arrangements mimicking magnetic spin textures, such as polar vortices and skyrmions, have been realized, but others, like helices of dipoles, have remained elusive. While earlier work claimed the presence of a helical dipole modulation in ferroelectric BiCu$_{x}$Mn$_{7-x}$O$_{12}$, our results rule out such a structure, motivating a renewed search for helical textures. Using atomic-resolution imaging, we report a novel form of helical order in which polar domains self-organize into a mesoscopic helical pattern: from domain to domain, polarization rotation follows a consistent handedness. Both right- and left-handed chirality emerging from this helical ordering are observed. This discovery establishes mesoscopic ordering as novel mechanism for inducing helical textures, and hence chirality, in ferroelectric crystals, paralleling the efforts in liquid crystals and supramolecular assemblies.

cond-mat.mes-hall↗

arXiv2025

Melting point depression of charge density wave in 1T-TiSe$_2$ due to size effects

Classical nucleation theory predicts size-dependent nucleation and melting due to surface and confinement effects at the nanoscale. In correlated electronic states, observation of size-dependent nucleation and melting is rarely reported, likely due to the extremely small length scales necessary to observe such effects for electronic states. Here, using 1T-TiSe$_2$ nanoflakes as a prototypical two-dimensional (2D) charge density wave (CDW) system, we perform in-situ cryogenic electron microscopy with temperature down to 20 K and observe size-dependent nucleation and melting of CDWs. Specifically, we observe a melting point depression of CDW for 1T-TiSe$_2$ flakes with lateral sizes less than 100 nm. By fitting experimental data to a Ginzburg-Landau model, we estimate a zero-temperature correlation length of 10--50 nm, which matches the reported CDW domain size for 1T-TiSe$_2$. As the flake size approaches the correlation length, the divergence of the CDW correlation length near the transition is cut off by the finite flake size, limiting long-range order and thereby lowering the transition temperature. For very small flakes whose size is close to the correlation length, we also observe absence of CDWs, as predicted by the model. We thus show that an electronic phase transition follows classical nucleation theory.

cond-mat.mtrl-sci↗

arXiv2025

Liquid Helium Cryogenic TEM below 1 Å

Next-generation cryogenic transmission electron microscopes (TEM) aim to achieve high-resolution imaging at ultracold sample temperatures (< 90 K) and over extended hold times. Lower temperatures enable atomic-scale characterization with improved beam and dose resilience for organic specimens and access to emergent electronic phases in quantum materials. Side-entry liquid helium cooling stages presently lack the mechanical and thermal stability required to support sub-Angstrom information transfer in modern TEM. Here we demonstrate sub-Angstrom atomic imaging TEM with a side-entry stage at specimen temperatures down to ~20K and with low stage drift and stable hold times.

physics.ins-det↗

arXiv2025

Real Space Visualization of Order-Disorder Transition in BaTiO3

Ferroelectricity in BaTiO3 was observed nearly eighty years ago, but the mechanism underlying its ferroelectric-paraelectric phase transition remains elusive. The order-disorder transition has been recognized as playing a critical role, however, the precise nature of the order parameter still remains under scrutiny, including the local dipole direction and the correlations above and below the Curie temperature. Using in situ scanning transmission electron microscopy, we directly map polar displacements in BaTiO3 across the ferroelectric-paraelectric phase transition, providing atomistic insights into a order-disorder mechanism. Atomic tracking reveals finite polar Ti displacements in the paraelectric phase where they manifest as random polar nanoregions. The displacements align along <111> direction in both the ferroelectric and paraelectric phases. The paraelectric-ferroelectric transition emerges from real-space correlations of the <111> polar Ti displacements. Our direct visualizations provides atomic insights into the order-disorder mechanism in the ferroelectric-paraelectric transition of BaTiO3.

cond-mat.mtrl-sci↗

arXiv2025

Topotactic oxidation of Ruddlesden-Popper nickelates reveals new structural family: oxygen-intercalated layered perovskites

Layered perovskites such as the Dion-Jacobson, Ruddlesden-Popper, and Aurivillius families host a wide range of correlated electron phenomena, from high-temperature superconductivity to multiferroicity. Here we report a new family of layered perovskites, realized through topotactic oxygen intercalation of La_{n+1}Ni_{n}O_{3n+1} (n=1-4) Ruddlesden-Popper nickelate thin films grown by ozone-assisted molecular-beam epitaxy. Post-growth ozone annealing induces a large c-axis expansion - 17.8% for La_{2}NiO_{4} (n=1) - that monotonically decreases with increasing n. Surface X-ray diffraction coupled with Coherent Bragg Rod Analysis reveals that this structural expansion arises from the intercalation of approximately 0.7 oxygen atoms per formula unit into interstitial sites within the rock salt spacer layers. The resulting structures exhibit a spacer layer composition intermediate between that of the Ruddlesden-Popper and Aurivillius phases, defining a new class of layered perovskites. Oxygen-intercalated nickelates exhibit metallicity and significantly enhanced nickel-oxygen hybridization, a feature linked to high-temperature superconductivity. Our work establishes topotactic oxidation as a powerful synthetic approach to accessing highly oxidized, metastable phases across a broad range of layered oxide systems, offering new platforms to tune properties via spacer-layer chemistry.

cond-mat.mtrl-sci↗

arXiv2025

Unconventional polaronic ground state in superconducting LiTi$_2$O$_4$

Geometrically frustrated lattices can display a range of correlated phenomena, ranging from spin frustration and charge order to dispersionless flat bands due to quantum interference. One particularly compelling family of such materials is the half-valence spinel Li$B_2$O$_4$ materials. On the $B$-site frustrated pyrochlore sublattice, the interplay of correlated metallic behavior and charge frustration leads to a superconducting state in LiTi$_2$O$_4$ and heavy fermion behavior in LiV$_2$O$_4$. To date, however, LiTi$_2$O$_4$ has primarily been understood as a conventional BCS superconductor despite a lattice structure that could host more exotic groundstates. Here, we present a multimodal investigation of LiTi$_2$O$_4$, combining ARPES, RIXS, proximate magnetic probes, and ab-initio many-body theoretical calculations. Our data reveals a novel mobile polaronic ground state with spectroscopic signatures that underlie co-dominant electron-phonon coupling and electron-electron correlations also found in the lightly doped cuprates. The cooperation between the two interaction scales distinguishes LiTi$_2$O$_4$ from other superconducting titanates, suggesting an unconventional origin to superconductivity in LiTi$_2$O$_4$. Our work deepens our understanding of the rare interplay of electron-electron correlations and electron-phonon coupling in unconventional superconducting systems. In particular, our work identifies the geometrically frustrated, mixed-valence spinel family as an under-explored platform for discovering unconventional, correlated ground states.

cond-mat.supr-con↗

arXiv2025

Inverse Melting of Polar Order in Chemically Substituted BaTiO3

In many condensed matter systems, long range order emerges at low temperatures as thermal fluctuations subside. In the presence of competing interactions or quenched disorder, however, some systems can show unusual configurations that become more disordered at low temperature, a rare phenomenon known as "inverse melting". Here, we discover an inverse melting of the polar order in a ferroelectric oxide with quenched chemical disorder (BaTi1-xZrxO3) through direct atomicscale visualization using in situ scanning transmission electron microscopy. In contrast to the clean BaTiO3 parent system in which long range order tracks lower temperatures, we observe in the doped system BaTi1-xZrxO3 that thermally driven fluctuations at high temperature give way to a more ordered state and then to a re-entrant disordered configuration at even lower temperature. Such an inverse melting of the polar order is likely linked to the random field generated by Zr dopants, which modulates the energy landscape arising from the competition between thermal fluctuations and random field pinning potential. These visualizations highlight a rich landscape of order and disorder in materials with quenched disorder, which may be key to understanding their advanced functionalities.

cond-mat.dis-nn↗

arXiv2024

Elastic plate basis for the deformation and electron diffraction of twisted bilayer graphene on a substrate

A basis is derived from elastic plate theory that quantifies equilibrium and dynamic deformation and electron diffraction patterns of twisted bilayer graphene (TBG). The basis is derived by solving in-plane and out-of-plane normal modes of an unforced parallelogram elastic plate. We show that a combination of only a few basis terms successfully captures the relaxed TBG structure with and without an underlying substrate computed using atomistic simulations. The results are validated by comparison with electron diffraction experiments. A code for extracting the elastic plate basis coefficients from an experimental electron diffraction image accompanies this paper. TBG dynamics are also studied by computing the phonon band structure from atomistic simulations. Low-energy phonons at the $Γ$ point are examined in terms of the mode shape and frequency. These modes are captured by simple elastic plate models with uniformly distributed springs for inter-layer and substrate interactions.

cond-mat.mtrl-sci↗

arXiv2024

Observation of stacking engineered magnetic phase transitions within moiré supercells of twisted van der Waals magnets

Twist engineering of magnetic van der Waals (vdW) moiré superlattices provides an attractive way to achieve precise nanoscale control over the spin degree of freedom on two-dimensional flatland. Despite the very recent demonstrations of moiré magnetism featuring exotic phases with noncollinear spin order in twisted vdW magnet chromium triiodide CrI3, the local magnetic interactions, spin dynamics, and magnetic phase transitions within and across individual moiré supercells remain elusive. Taking advantage of a scanning single-spin magnetometry platform, here we report observation of two distinct magnetic phase transitions with separate critical temperatures within a moiré supercell of small-angle twisted double trilayer CrI3. By measuring temperature dependent spin fluctuations at the coexisting ferromagnetic and antiferromagnetic regions in twisted CrI3, we explicitly show that the Curie temperature of the ferromagnetic state is higher than the Néel temperature of the antiferromagnetic one by ~10 K. Our mean-field calculations attribute such a spatial and thermodynamic phase separation to the stacking order modulated interlayer exchange coupling at the twisted interface of the moiré superlattices. The presented results highlight twist engineering as a promising tuning knob to realize on-demand control of not only the nanoscale spin order of moiré quantum matter but also its dynamic magnetic responses, which may find relevant applications in developing transformative vdW electronic and magnetic devices.

cond-mat.mes-hall↗

arXiv2024

Ultra-Cold Cryogenic TEM with Liquid Helium and High Stability

Cryogenic transmission electron microscopy has revolutionized structural biology and materials science, but achieving temperatures below the boiling point of liquid nitrogen remains a long-standing aspiration. We introduce an ultra-cold liquid helium transmission electron microscope specimen holder, featuring continuous cryogen flow and vibration decoupling. This instrument is compatible with modern aberration-corrected microscopes and achieves sub-25 K base temperature, ${\pm}$2 mK thermal stability over many hours, and atomic resolution--setting the stage for a new era of cryogenic electron microscopy.

physics.app-ph↗

arXiv2023

"Extraordinary" Phase Transition Revealed in a van der Waals Antiferromagnet

While the surface-bulk correspondence has been ubiquitously shown in topological phases, the relationship between surface and bulk in Landau-like phases is much less explored. Theoretical investigations since 1970s for semi-infinite systems have predicted the possibility of the surface order emerging at a higher temperature than the bulk, clearly illustrating a counterintuitive situation and greatly enriching phase transitions. But experimental realizations of this prediction remain missing. Here, we demonstrate the higher-temperature surface and lower-temperature bulk phase transitions in CrSBr, a van der Waals (vdW) layered antiferromagnet. We leverage the surface sensitivity of electric dipole second harmonic generation (SHG) to resolve surface magnetism, the bulk nature of electric quadrupole SHG to probe bulk spin correlations, and their interference to capture the two magnetic domain states. Our density functional theory calculations show the suppression of ferromagnetic-antiferromagnetic competition at the surface responsible for this enhanced surface magnetism. Our results not only show unexpected, richer phase transitions in vdW magnets, but also provide viable ways to enhance magnetism in their 2D form.

cond-mat.mtrl-sci↗

arXiv2023

Endotaxial Stabilization of 2D Charge Density Waves with Long-range Order

Charge density waves are emergent quantum states that spontaneously reduce crystal symmetry, drive metal-insulator transitions, and precede superconductivity. In low-dimensions, distinct quantum states arise, however, thermal fluctuations and external disorder destroy long-range order. Here we stabilize ordered two-dimensional (2D) charge density waves through endotaxial synthesis of confined monolayers of 1T-TaS$_2$. Specifically, an ordered incommensurate charge density wave (oIC-CDW) is realized in 2D with dramatically enhanced amplitude and resistivity. By enhancing CDW order, the hexatic nature of charge density waves becomes observable. Upon heating via in-situ TEM, the CDW continuously melts in a reversible hexatic process wherein topological defects form in the charge density wave. From these results, new regimes of the CDW phase diagram for 1T-TaS$_2$ are derived and consistent with the predicted emergence of vestigial quantum order.

cond-mat.mtrl-sci↗

arXiv2023

Revealing intrinsic domains and fluctuations of moiré magnetism by a wide-field quantum microscope

Moiré magnetism featured by stacking engineered atomic registry and lattice interactions has recently emerged as an appealing quantum state of matter at the forefront condensed matter physics research. Nanoscale imaging of moiré magnets is highly desirable and serves as a prerequisite to investigate a broad range of intriguing physics underlying the interplay between topology, electronic correlations, and unconventional nanomagnetism. Here we report spin defect-based wide-field imaging of magnetic domains and spin fluctuations in twisted double trilayer (tDT) chromium triiodide CrI3. We explicitly show that intrinsic moiré domains of opposite magnetizations appear over arrays of moiré supercells in low-twist-angle tDT CrI3. In contrast, spin fluctuations measured in tDT CrI3 manifest little spatial variations on the same mesoscopic length scale due to the dominant driving force of intralayer exchange interaction. Our results enrich the current understanding of exotic magnetic phases sustained by moiré magnetism and highlight the opportunities provided by quantum spin sensors in probing microscopic spin related phenomena on two-dimensional flatland.

cond-mat.mes-hall↗