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Heemin Lee

Publications and source records attributed to Heemin Lee.

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Low-Temperature Suppression of Intertwined Orders in La$_{1/3}$Sr$_{2/3}$FeO$_{3}$ Thin Films

The strong coupling between spin, charge, and lattice degrees of freedom in perovskite oxides leads to an array of exotic phenomena, giving these materials rich phase diagrams that can include coupled orders. This is exemplified by the A-site doped ferrite La$_{1/3}$Sr$_{2/3}$FeO$_{3}$ (LSFO), which exhibits a coupled paramagnetic-antiferromagnetic and charge ordering phase transition at $\sim$190 K that has been well studied in thin films, bulk, and polycrystalline samples. However, the low temperature behavior of LSFO thin films below $\sim$100 K has not been thoroughly explored. This work uses several X-ray scattering and spectroscopy techniques to directly probe LSFO's magnetic and charge order down to low temperature. Using resonant X-ray scattering, we observe a complete suppression of LSFO's known antiferromagnetic and charge order below $\sim$25 K. Further spectroscopy and coherent scattering measurements provide insight into LSFO's electronic structure and domain dynamics in this new low temperature phase, and we propose possible explanations for the observed order suppression based on reduced dimensionality of domains in our thin films. Our findings provide insight into the effects of competing interactions in strongly correlated materials, particularly those with coupled orders.

cond-mat.str-el

Interlayer Five-Spin Polaron in Superconducting Bilayer Nickelates

The discovery of high-$T_c$ superconductivity in Ruddlesden-Popper nickelates has sparked substantial effort towards understanding unconventional electronic states beyond a traditional cuprate-like $d^9$ configurational ground state. An understanding of the interplay between magnetic ground states and multi-orbital physics is key for establishing a microscopic mechanism for superconductivity. In the bilayer nickelates, spin density wave (SDW) order is a prominent feature in the non-superconducting regime, yet its relation to superconducting pairing remains an open question. Here, we use resonant x-ray scattering to examine the existence of SDW order in superconducting bilayer nickelate thin films La$_2$PrNi$_2$O$_7$ (LPNO). Comparing superconducting and oxygen-deficient LPNO thin films, we find that superconductivity occurs in SDW-free, oxygen-stoichiometric regions, whereas oxygen-deficiency promotes SDW order, indicating phase segregation of SDW and superconductivity. Furthermore, Ni-$L_3$ and O-$K$ edge spectroscopy reveals distinct electronic structures - particularly along the $c$-axis - between the two regions. Our results identify oxygen stoichiometry as a key parameter controlling interlayer coupling and thus the electronic structure of bilayer nickelates. In concert with theory, we propose that a ligand hole primarily resides at the inter-bilayer apical oxygen, forming a robust interlayer five-spin polaron state, which serves as the ground state for superconducting bilayer nickelates.

cond-mat.str-el

Long-range magnetic order with disordered spin orientations in a high-entropy antiferromagnet

Disorder in magnetic systems typically suppresses long-range order, promoting short-range states such as spin glasses and magnetic clusters. This is particularly prominent in high-entropy materials, characterized by the random distributions of local magnetic entities and exchange interactions. However, in rare exceptions, long-range magnetic order can persist in high-entropy systems, while the microscopic characters and underlying mechanisms remain elusive, especially the magnetic behaviors of individual elements. Here, combining neutron diffraction and resonant soft x-ray scattering, we have conducted an element-specific investigation into the magnetic order of a high-entropy honeycomb-lattice van der Waals material (Mn1/4Fe1/4Co1/4Ni1/4)PS3. Despite significant atomic disorder, long-range zigzag antiferromagnetic order is observed below 72 K, with all four transition-metal elements participating in a unified phase transition. However, the spin orientations of various elements are distinct, attributed to the competition between single-ion anisotropies and exchange interactions. Our findings showcase a novel form of long-range magnetic order with disordered spin orientations, which is synergically stabilized by distinct magnetic elements in a high entropy magnet, offering a new paradigm for understanding complex magnetic systems.

cond-mat.str-el

Probing Coordination Environments in Buried Oxides of Aluminum Josephson Junctions by Resonant X-ray Reflectivity

Decoherence remains a critical obstacle to achieving high-fidelity, scalable superconducting qubits, with the tunnel barrier of Josephson junctions a key source of loss. Here we apply resonant X-ray reflectivity to non-destructively probe the electronic structure of buried layers in Al/AlO$_x$/Al Josephson junctions. At the Al $K$-edge, energy-dependent modulations in the reflectivity maps enable Kramers-Kronig-constrained extraction of the layer-resolved atomic scattering factors. The analysis reveals that the barrier coordination evolves from more tetrahedral toward predominantly octahedral character with increasing oxidation pressure. At the interfaces, the lower metal-oxide boundary is comparatively under-coordinated and disordered relative to the upper interface. Comparison with simulated X-ray absorption spectra identifies the dominant coordination motifs within the oxide and its interfaces, providing depth-resolved structural insight that constrains microscopic models of two-level system formation. These results link growth conditions, local coordination environments, and junction electronic properties, demonstrating resonant X-ray reflectivity as a powerful tool for probing the microscopic materials properties of Josephson junctions and providing a materials-level framework for mitigating decoherence in superconducting qubits.

cond-mat.mtrl-sci

Introducing new resonant soft x-ray scattering capability in SSRL

Resonant soft X-ray scattering (RSXS) is a powerful technique for probing both spatial and electronic structures within solid-state systems. We present a newly developed RSXS capability at beamline 13-3 of the Stanford Synchrotron Radiation Lightsource (SSRL), designed to enhance materials science research. This advanced setup achieves a base sample temperature as low as 9.8 K combined with extensive angular motions (azimuthal \phi and flipping \chi), enabling comprehensive exploration of reciprocal space. Two types of detectors, an Au/GaAsP Schottky photodiode and a CCD detector with over 95% quantum efficiency, are integrated to effectively capture scattered photons. Extensive testing has confirmed the enhanced functionality of this RSXS setup, including its temperature and angular performance. The versatility and effectiveness of the system have been demonstrated through studies of various materials, including superlattice heterostructures and high-temperature superconductors.

physics.ins-det

Hidden dormant phase mediating the glass transition in disordered matter

Metallic glass is a frozen liquid with structural disorder that retains degenerate free energy without spontaneous symmetry breaking to become a solid. For over half a century, this puzzling structure has raised fundamental questions about how structural disorder impacts glass-liquid phase transition kinetics, which remain elusive without direct evidence. In this study, through single-pulse, time-resolved imaging using X-ray free-electron lasers, we visualized the glass-to-liquid transition, revealing a previously hidden dormant phase that does not involve any macroscopic volume change within the crossover regime between the two phases. Although macroscopically inactive, nanoscale redistribution occurs, forming channeld low-density bands within this dormant phase that drives the glass transition. By providing direct microscopic evidence, this work presents a new perspective on the phase transition process in disordered materials, which can be extended to various liquid and solid phases in other complex systems.

cond-mat.dis-nn

Photoinduced surface plasmon control of ultrafast melting modes in Au nanorods

Photoinduced ultrafast phenomena in materials exhibiting nonequilibrium behavior can lead to the emergence of exotic phases beyond the limits of thermodynamics, presenting opportunities for femtosecond photoexcitation. Despite extensive research, the ability to actively control quantum materials remains elusive owing to the lack of clear evidence demonstrating the explicit control of phase-changing kinetics through light-matter interactions. To address this drawback, we leveraged single-pulse time-resolved X-ray imaging of Au nanorods undergoing photoinduced melting to showcase control over the solid-to-liquid transition process through the use of localized surface plasmons. Our study uncovers transverse or longitudinal melting processes accompanied by characteristic oscillatory distortions at different laser intensities. Numerical simulations confirm that the localized surface plasmons, excited by polarized laser fields, dictate the melting modes through anharmonic lattice deformations. These results provide direct evidence of photoinduced surface plasmon-mediated ultrafast control of matter, establishing a foundation for the customization of material kinetics using femtosecond laser fields.

cond-mat.mes-hall

Frustrated phonon with charge density wave in vanadium Kagome metal

The formation of a star of David CDW superstructure, resulting from the coordinated displacements of vanadium ions on a corner sharing triangular lattice, has garnered significant attention to comprehend the influence of electron phonon interaction within geometrically intricate lattice of Kagome metals, specifically AV3Sb5 (where A represents K, Rb, or Cs). However, understanding of the underlying mechanism behind CDW formation, coupled with symmetry protected lattice vibrations, remains elusive. Here, from femtosecond time resolved X ray scattering experiments, we reveal that the phonon mode, associated with Cs ions out-of-plane motion, becomes frustrated in the CDW phase. Furthermore, we observed the photoinduced emergence of a metastable CDW phase, facilitated by alleviating the frustration. By not only elucidating the longstanding puzzle surrounding the intervention of phonons but introducing the phononic frustration, this research offers fresh insights into the competition between phonons and periodic lattice distortions, a phenomenon widespread in other correlated quantum materials including layered high TC superconductors.

cond-mat.str-el

Observation of Subharmonic Charge-Density-Wave Correlations in La-Based Cuprates

Pair-density-wave (PDW) correlations have been proposed as an important ingredient in the complex phase diagram of high-$T_{\rm c}$ cuprates, yet bulk-sensitive experimental signatures remain scarce. Here we report resonant x-ray scattering measurements revealing a subharmonic charge-density-wave (CDW) scattering response in Sr-doped $1/8$-LBCO. The subharmonic response appears at approximately half the primary CDW ordering wave vector and emerges within a physically relevant temperature regime associated with the development of in-plane superconducting correlations. Comparable subharmonic behavior is also observed in a chemically distinct La-based cuprate, LSCO, within the same stripe-ordered, layer-decoupled regime. Together, these observations identify a bulk-sensitive scattering signature that is consistent with PDW correlations in La-based superconducting cuprates.

cond-mat.supr-con

High-throughput ensemble characterization of individual core-shell nanoparticles with quantitative 3D density from XFEL single-particle imaging

The structures, as building-blocks for designing functional nanomaterials, have fueled the development of versatile nanoprobes to understand local structures of noncrystalline specimens. Progresses in analyzing structures of individual specimens with atomic scale accuracy have been notable recently. In most cases, however, only a limited number of specimens are inspected lacking statistics to represent the systems with structural inhomogeneity. Here, by employing single-particle imaging with X-ray free electron lasers and new algorithm for multiple-model 3D imaging, we succeeded in investigating several thousand specimens in a couple of hours, and identified intrinsic heterogeneities with 3D structures. Quantitative analysis has unveiled 3D morphology, facet indices and elastic strains. The 3D elastic energy distribution is further corroborated by molecular dynamics simulations to gain mechanical insight at atomic level. This work establishes a new route to high-throughput characterization of individual specimens in large ensembles, hence overcoming statistical deficiency while providing quantitative information at the nanoscale.

cond-mat.mtrl-sci