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Kim, Sungwon

Publications and source records attributed to Kim, Sungwon.

X-ray induced grain boundary formation and grain rotation in Bi 2 Se 3

Optimizing grain boundary characteristics in polycrystalline materials can improve their properties. Many processing methods have been developed for grain boundary manipulation, including the use of intense radiation in certain applications. Here, in this work, we used X-ray free electron laser pulses to irradiate single-crystalline bismuth selenide (Bi 2 Se 3 ) and observed grain boundary formation and subsequent grain rotation in response to the X-ray radiation. Our observations with simultaneous transmission X-ray microscopy and X-ray diffraction demonstrate how intense X-ray radiation can rapidly change size and texture of grains.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Emergence of liquid following laser melting of gold thin films

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.

36 MATERIALS SCIENCE↗

Simultaneous bright- and dark-field X-ray microscopy at X-ray free electron lasers

Abstract The structures, strain fields, and defect distributions in solid materials underlie the mechanical and physical properties across numerous applications. Many modern microstructural microscopy tools characterize crystal grains, domains and defects required to map lattice distortions or deformation, but are limited to studies of the (near) surface. Generally speaking, such tools cannot probe the structural dynamics in a way that is representative of bulk behavior. Synchrotron X-ray diffraction based imaging has long mapped the deeply embedded structural elements, and with enhanced resolution, dark field X-ray microscopy (DFXM) can now map those features with the requisite nm-resolution. However, these techniques still suffer from the required integration times due to limitations from the source and optics. This work extends DFXM to X-ray free electron lasers, showing how the $$10^{12}$$ 10 12 photons per pulse available at these sources offer structural characterization down to 100 fs resolution (orders of magnitude faster than current synchrotron images). We introduce the XFEL DFXM setup with simultaneous bright field microscopy to probe density changes within the same volume. This work presents a comprehensive guide to the multi-modal ultrafast high-resolution X-ray microscope that we constructed and tested at two XFELs, and shows initial data demonstrating two timing strategies to study associated reversible or irreversible lattice dynamics.

47 OTHER INSTRUMENTATION↗

Strain and crystallographic identification of the helically concaved gap surfaces of chiral nanoparticles

Identifying the three-dimensional (3D) crystal plane and strain-field distributions of nanocrystals is essential for optical, catalytic, and electronic applications. However, it remains a challenge to image concave surfaces of nanoparticles. Here, we develop a methodology for visualizing the 3D information of chiral gold nanoparticles ≈ 200 nm in size with concave gap structures by Bragg coherent X-ray diffraction imaging. The distribution of the high-Miller-index planes constituting the concave chiral gap is precisely determined. The highly strained region adjacent to the chiral gaps is resolved, which was correlated to the 432-symmetric morphology of the nanoparticles and its corresponding plasmonic properties are numerically predicted from the atomically defined structures. This approach can serve as a comprehensive characterization platform for visualizing the 3D crystallographic and strain distributions of nanoparticles with a few hundred nanometers, especially for applications where structural complexity and local heterogeneity are major determinants, as exemplified in plasmonics.

36 MATERIALS SCIENCE↗

Ultrafast Carrier–Lattice Interactions and Interlayer Modulations of Bi 2 Se 3 by X-ray Free-Electron Laser Diffraction

We report as a 3D topological insulator, bismuth selenide (Bi 2 Se 3 ) has potential applications for electrically and optically controllable magnetic and optoelectronic devices. Understanding the coupling with its topological phase requires studying the interactions of carriers with the lattice on time scales down to the sub-picosecond regime. Here we investigate the ultrafast carrier-induced lattice contractions and interlayer modulations in Bi 2 Se 3 thin films by time-resolved diffraction using an X-ray free-electron laser. The lattice contraction depends on the carrier concentration and is followed by an interlayer expansion accompanied by oscillations. Using density functional theory (DFT) and the Lifshitz model, the initial contraction can be explained by van der Waals force modulation of the confined free carrier layers. Our theory suggests that band inversion, related to a topological phase transition, is modulated by the expansion of the interlayer distance. These results provide insights into the topological phase control by light-induced structural change on ultrafast timescales.

77 NANOSCIENCE AND NANOTECHNOLOGY↗

In Situ Strain Evolution on Pt Nanoparticles during Hydrogen Peroxide Decomposition

Fundamental understanding of structural changes during catalytic reactions is crucial to understanding the underlying mechanisms and optimizing efficiencies. Surface energy and related catalytic mechanisms are widely studied. However, the catalyst lattice deformation induced by catalytic processes is not well understood. Here, we study the strain in an individual platinum (Pt) nanoparticle (NP) using Bragg coherent diffraction imaging under in situ oxidation and reduction reactions. When Pt NPs are exposed to H 2 O 2 , a typical oxidizer and an intermediate during the oxygen reduction reaction process, alternating overall strain distribution near the surface and inside the NP is observed at the (111) Bragg reflection. In contrast, relatively insignificant changes appear in the (200) reflection. Density functional theory calculations are employed to rationalize the anisotropic lattice strain in terms of induced stress by H 2 O 2 adsorption and decomposition on the Pt NP surface. Our study provides deeper insight into the activity-structure relationship in this system.

3D imaging↗