Heemin Lee

Decoherence remains a critical obstacle to achieving high-fidelity, scalable superconducting qubits, with the tunnel barrier of Josephson junctions a key source of loss, yet the microscopic structure of this buried layer has remained difficult to probe experimentally. Here, we use resonant x-ray reflectivity to resolve the coordination environments within the AlO x barrier of Al / AlO x / Al Josephson junctions as a function of oxidation conditions. We find that the barrier coordination evolves from more tetrahedral toward octahedral character with increasing oxidation pressure, while the lower metal-oxide interface is comparatively undercoordinated and disordered relative to the upper interface. Comparison with simulated x-ray absorption spectra identifies the dominant coordination motifs within the oxide and at its interfaces, providing depth-resolved structural insight that informs microscopic models of two-level system formation. These results link growth conditions, local coordination environments, and junction electronic properties, providing a materials-level foundation for interpreting how the tunnel barrier influences coherence in superconducting qubits.

For decades, superconductivity in high-T_{c} cuprates has been viewed as a competitor that suppresses charge-density-wave (CDW) order by reducing its amplitude and spatial extent. Here, we show that this picture is incomplete, as superconductivity is accompanied by a systematic enhancement of CDW phase coherence across multiple cuprate families. Using resonant soft x-ray scattering combined with a coherence-sensitive momentum-profile analysis, we uncover a BCS-like growth of phase coherence below T_{c}, which phenomenologically manifests as the absence of CDW peak broadening and near-perfect wave-vector locking. This enhancement remains visible even in a disorder-dominated regime created by long-term crystal aging and follows a common trend when compared with published data on Bi-, Hg-, Y-, and Nd-based cuprates. These results indicate that superconductivity reshapes CDW order in two distinct ways, suppressing its amplitude while strengthening its phase coherence, and reveal an additional phase-level interplay with lattice coupling in high-T_{c} cuprates.

The infinite-layer compound CaCoO 2 provides a compelling platform to explore how local orbital distortions evolve into collective electronic order. Using resonant soft x-ray scattering (RSXS) and its time-resolved counterpart (tr-RSXS), we reveal a cooperative coupling between two intertwined orders at the same in-plane wave vector, q ≈ ( 1 / 4 , 1 / 4 , 0 ) , comprising a quasi-two-dimensional orbital order associated with the distorted Co ( 1 ) sites and a quasi-three-dimensional trimerlike charge order stabilized through Co-O-Ca hybridization. The charge-sensitive component exhibits a uniform relaxation time of ∼ 400 fs ( 391 ± 5 fs ) across multiple Co resonances, evidencing a collective charge response. A comparable timescale observed in the orbital order associated with the highly distorted Co ( 1 ) sites indicates that this collective behavior naturally originates from the same orbital framework that mediates both charge and orbital degrees of freedom. Together, these findings establish CaCoO 2 as a model system in which Jahn-Teller distortions, orbital hybridization, and geometric frustration cooperate to form molecular trimer units that dictate the macroscopic electronic behavior.

Ultrafast laser excitation can drive materials into exotic states beyond thermodynamic limits, offering alternative ways to control how matter stores and releases energy. Yet, whether light can actively steer energy-relaxation pathways during structural transitions remains unclear due to the lack of direct experimental evidence. Here we show, using single-pulse time-resolved X-ray imaging of gold nanorods, that photoinduced localized surface plasmons control ultrafast energy relaxation into distinct deformation modes, transverse or longitudinal deformation modes, each accompanied by characteristic plasmon-induced oscillatory distortions depending on the laser fluence. Numerical simulations further confirm that localized surface plasmons dictate ultrafast energy relaxation process from photoexcited hot electrons to anharmonic nanocrystal deformations. Our results provide direct evidence that surface plasmon-mediated interactions enable ultrafast, nanoscale control of materials’ energetics, opening a pathway for tailoring energy-transfer processes with femtosecond laser fields. This approach lays the foundation for customizing nonequilibrium phase dynamics at the nanoscale and provides a route to tailoring energy-transfer processes using femtosecond laser fields.

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, 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 ϕ and flipping χ), enabling comprehensive exploration of reciprocal space. Two types of detectors—an Au/GaAsP Schottky photodiode and a charge-coupled device 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.

The formation of a star-of-David charge density wave 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 charge density wave 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 cesium ions’ out-of-plane motion, becomes frustrated in the charge density wave phase. Furthermore, we observed the photoinduced emergence of a metastable charge density wave 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 insights into the competition between phonons and periodic lattice distortions, a phenomenon widespread in other correlated quantum materials including layered high-temperature superconductors.

Ultrafast photoinduced melting provides an essential platform for studying nonequilibrium phase transitions by linking the kinetics of electron dynamics to ionic motions. Knowledge of dynamic balance in their energetics is essential to understanding how the ionic reaction is influenced by femtosecond photoexcited electrons with notable time lag depending on reaction mechanisms. Here, by directly imaging fluctuating density distributions and evaluating the ionic pressure and Gibbs free energy from two-temperature molecular dynamics that verified experimental results, we uncovered that transient ionic pressure, triggered by photoexcited electrons, controls the overall melting kinetics. In particular, ultrafast nonequilibrium melting can be described by the reverse nucleation process with voids as nucleation seeds. The strongly driven solid-to-liquid transition of metallic gold is successfully explained by void nucleation facilitated by photoexcited electron–initiated ionic pressure, establishing a solid knowledge base for understanding ultrafast nonequilibrium kinetics.

X-ray structural science is undergoing a revolution driven by the emergence of X-ray Free-electron Laser (XFEL) facilities. The structures of crystalline solids can now be studied on the picosecond time scale relevant to phonons, atomic vibrations which travel at acoustic velocities. In the work presented here, X-ray diffuse scattering is employed to characterize the time dependence of the liquid phase emerging from femtosecond laser-induced melting of polycrystalline gold thin films using an XFEL. In a previous analysis of Bragg peak profiles, we showed the supersonic disappearance of the solid phase and presented a model of pumped hot electrons carrying energy from the gold surface to scatter at internal grain boundaries. This generates melt fronts propagating relatively slowly into the crystal grains. By conversion of diffuse scattering to a partial X-ray pair distribution function, we demonstrate that it has the characteristic shape obtained by Fourier transformation of the measured F(Q). The diffuse signal fraction increases with a characteristic rise-time of 13 ps, roughly independent of the incident pump fluence and consequent final liquid fraction. This suggests the role of further melt-front nucleation processes beyond grain boundaries.

Photoinduced nonequilibrium phase transitions have stimulated interest in the dynamic interactions between electrons and crystalline ions, which have long been overlooked within the Born–Oppenheimer approximation. Ultrafast melting before lattice thermalization prompted researchers to revisit this issue to understand ultrafast photoinduced weakening of the crystal bonding. However, the absence of direct evidence demonstrating the role of orbital dynamics in lattice disorder leaves it elusive. By performing time-resolved resonant X-ray scattering with an X-ray free-electron laser, we directly monitored the ultrafast dynamics of bonding orbitals of Ge to drive photoinduced melting. Increased photoexcitation of bonding electrons amplifies the orbital disturbance to expedite the lattice disorder approaching the sub-picosecond scale of the nonthermal regime. The lattice disorder time shows strong nonlinear dependence on the laser fluence with a crossover behavior from thermal-driven to nonthermal-dominant kinetics, which is also verified by ab initio and two-temperature molecular dynamics simulations. This study elucidates the impact of bonding orbitals on lattice stability with a unifying interpretation on photoinduced melting.

With the advent of x-ray free electron lasers (XFELs), ultrafast laser excitation leading to nonequilibrium states has become an important way to investigate thermal processes. Here, we use ultrafast x-ray diffraction in an XFEL pump-probe experiment to examine the lattice dynamics of 300 nm polycrystalline palladium (Pd) thin films. In our experiment, at higher laser fluence levels, we directly observe a compression effect launched from the surface skin layer heated by the optical pulse which propagates across the film over the first tens of picoseconds. After that, a lattice expansion becomes dominant, followed by a quasi-steady state lasting into the nanosecond timescale. For the lowest fluence, the compression component is not detected, indicating that the dynamics is highly dependent on the laser power. Our results shed light on the dynamics behind ultrafast processes in metallic Pd, and they can be extended to different crystalline structures.