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Hyunjung Kim

Publications and source records attributed to Hyunjung Kim.

10 recordsLinked to original sources

Cumulative X-ray Damage in Bismuth Selenide Examined by Simultaneous TXM and XRD

Bismuth selenide (Bi2Se3) is a topological insulator with potential applications in thermoelectrics, spintronics, and optoelectronics. However, its response to radiation remains poorly understood. We investigate cumulative X-ray damage in Bi2Se3 using simultane- ous transmission X-ray microscopy (TXM) and X-ray diffraction (XRD) at the Pohang Accelerator Laboratory X-Ray Free Electron Laser (PAL-XFEL) over 27,000 successive pulses. We observe distinct damage mechanisms: rapid hole formation via vaporization within 100 pulses, followed by slower grain refinement and material sputtering over thousands of thermal cycles. Williamson-Hall analysis reveals a progressive transformation from single-crystal to nanocrystalline structure, with grain sizes decreasing from mi- cron to nanometer scale. Finite-element modeling confirms that X-rays penetrate 13.47 μm, driving local temperatures above 1600 K with subsequent cooling between pulses. Scanning electron microscopy identifies three characteristic morphologies correspond- ing to different thermal histories: sputter streaks, prismatic crystals, and disordered microcrystals. Our results demonstrate that grain-boundary formation creates a feedback mechanism that accelerates damage in later pulses. This work establishes a method- ology for studying radiation damage across multiple length scales and provides insight into topological insulator stability under extreme conditions

cond-mat.mtrl-sci

Atomically Resolved Acoustic Dynamics Coupled with Magnetic Order in a van der Waals Antiferromagnet

Magnetoelastic coupling in van der Waals (vdW) magnetic materials enables a unique interplay between the spin and lattice degrees of freedom. Characterizing the elastic responses with atomic and femtosecond resolution across the magnetic transition is essential for guiding the design of magnetically tunable actuators and strain-mediated spintronic devices. Here, ultrafast x-ray diffraction employed at a free-electron laser reveals that the atomic displacements, wave vectors, and dispersion relations of acoustic phonon modes in a vdW antiferromagnet FePS$_3$ are coupled with the magnetic order, by tracking both in-plane and out-of-plane Bragg peaks upon optical excitation across the Néel temperature (T$_N$). One transverse mode shows that a quasi-out-of-plane atomic displacement undergoes a significant directional change across T$_N$. Its quasi-in-plane wave vector is derived by the comparison between the measured sound velocity and the first-principles calculations. The other transverse mode is an interlayer shear acoustic mode whose amplitude is strongly enhanced in the antiferromagnetic phase, exhibiting eight times stronger amplitude than the longitudinal acoustic mode below T$_N$. The atomically resolved characterization of acoustic phonon dynamics that couple with magnetic ordering opens opportunities for harnessing unique magnetoelastic coupling in vdW magnets on ultrafast timescales.

cond-mat.mtrl-sci

Low temperature state in strontium titanate microcrystals using in situ multi-reflection Bragg coherent X-ray diffraction imaging

Strontium titanate is a classic quantum paraelectric oxide material that has been widely studied in bulk and thin films. It exhibits a well-known cubic-to-tetragonal antiferrodistortive phase transition at 105 K, characterized by the rotation of oxygen octahedra. A possible second phase transition at lower temperature is suppressed by quantum fluctuations, preventing the onset of ferroelectric order. However, recent studies have shown that ferroelectric order can be established at low temperatures by inducing strain and other means. Here, we used in situ multi-reflection Bragg coherent x-ray diffraction imaging to measure the strain and rotation tensors for two strontium titanate microcrystals at low temperature. We observe strains induced by dislocations and inclusion-like impurities in the microcrystals. Based on radial magnitude plots, these strains increase in magnitude and spread as the temperature decreases. Pearson's correlation heat maps show a structural transition at 50 K, which could possibly be the formation of a low-temperature ferroelectric phase in the presence of strain. We do not observe any change in local strains associated with the tetragonal phase transition at 105 K.

cond-mat.mtrl-sci

X-ray induced grain boundary formation and grain rotation in Bi2Se3

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. In this work, we used X-ray free electron laser pulses to irradiate single-crystalline bismuth selenide (Bi2Se3) 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.

cond-mat.mtrl-sci

Simultaneous Bright- and Dark-Field X-ray Microscopy at X-ray Free Electron Lasers

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 $10^{12}$ 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.

cond-mat.mtrl-sci

Ultrafast X-ray imaging of the light-induced phase transition in VO2

Using light to control transient phases in quantum materials is an emerging route to engineer new properties and functionality, with both thermal and non-thermal phases observed out of equilibrium. Transient phases are expected to be heterogeneous, either through photo-generated domain growth or by generating topological defects, and this impacts the dynamics of the system. However, this nanoscale heterogeneity has not been directly observed. Here we use time- and spectrally resolved coherent X-ray imaging to track the prototypical light induced insulator-to-metal phase transition in vanadium dioxide on the nanoscale with femtosecond time resolution. We show that the early-time dynamics are independent of the initial spatial heterogeneity and observe a 200 fs switch to the metallic phase. A heterogeneous response emerges only after hundreds of picoseconds. Through spectroscopic imaging, we reveal that the transient metallic phase is a highly orthorhombically strained rutile metallic phase, an interpretation that is in contrast to those based on spatially averaged probes. Our results demonstrate the critical importance of spatially and spectrally resolved measurements for understanding and interpreting the transient phases of quantum materials.

cond-mat.str-el

Strain and Crystallographic Identification of the Helically Concaved Surfaces of Nanoparticles

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

cond-mat.mtrl-sci

Ultrafast carrier-lattice interactions and interlayer modulations of Bi2Se3 by X-ray free electron laser diffraction

As a 3D topological insulator, bismuth selenide (Bi2Se3) has potential applications for electrically and optically controllable magnetic and optoelectronic devices. How the carriers interact with lattice is important to understand the coupling with its topological phase. It is essential to measure with a time scale smaller than picoseconds for initial interaction. Here we use an X-ray free-electron laser to perform time-resolved diffraction to study ultrafast carrier-induced lattice contractions and interlayer modulations in Bi2Se3 thin films. 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. Band inversion, related to a topological phase transition, is modulated by the expansion of the interlayer distance. These results provide insight into instantaneous topological phases on ultrafast timescales.

cond-mat.mtrl-sci

Persistence of Island Arrangements During Layer-by-Layer Growth Revealed Using Coherent X-rays

Understanding surface dynamics during epitaxial film growth is key to growing high quality materials with controllable properties. X-ray photon correlation spectroscopy (XPCS) using coherent x-rays opens new opportunities for in situ observation of atomic-scale fluctuation dynamics during crystal growth. Here, we present the first XPCS measurements of 2D island dynamics during homoepitaxial growth in the layer-by-layer mode. Analysis of the results using two-time correlations reveals a new phenomenon - a memory effect in island nucleation sites on successive crystal layers. Simulations indicate that this persistence in the island arrangements arises from communication between islands on different layers via adatoms. With the worldwide advent of new coherent x-ray sources, the XPCS methods pioneered here will be widely applicable to atomic-scale processes on surfaces.

cond-mat.mtrl-sci

Characteristics of Nickel Thin Film and Formation of Nickel Silicide by Remote Plasma Atomic Layer Deposition using Ni(iPr-DAD)2

In this study, the characteristics of nickel thin film deposited by remote plasma atomic layer deposition (RPALD) on p-type Si substrate and formation of nickel silicide using rapid thermal annealing were determined. Bis(1,4-di-isopropyl-1,3-diazabutadienyl)nickel, Ni(iPr-DAD)2, was used as a Ni precursor and ammonia plasma was used as a reactant. This was the first attempt to deposit Ni thin film using Ni(iPr-DAD)2 as a precursor for the ALD process. The RPALD Ni film was deposited with a growth rate of around 2.2Å/cycle at 250 °C and showed significant low resistivity of 33 μΩcm with a total impurity concentration of around 10 at. %.The impurities of the thin film, carbon and nitrogen, were existent by the forms of C-C and C-N in a bonding state. The impurities removal tendency was investigated by comparing of experimental conditions, namely process temperature and pressure. Nitrogen impurity was removed by thermal desorption during each ALD cycle and carbon impurity was reduced by the optimizing of the process pressure which is directly related with a mean free path of NH3 plasma. After Ni deposition, nickel silicide was formed by RTA in a vacuum ambient for 1 minute. A nickel silicide layer from ALD Ni and PVD Ni was compared at the annealing temperature from 500 to 900 °C. NiSi from ALD Ni showed better thermal stability due to the contribution of small amounts of carbon and nitrogen in the asdeposited Ni thin film. Degradation of the silicide layer was effectively suppressed with a use of ALD Ni.

cond-mat.mtrl-sci