arXiv subjects

Peihao Sun

Publications and source records attributed to Peihao Sun.

13 recordsLinked to original sources

arXiv2026

Crystallisation kinetics of supercooled liquid palladium

In this study, we employ classical molecular dynamics (MD) simulations to investigate the crystallisation kinetics of supercooled liquid palladium and relate the results to time-resolved X-ray diffraction measurements on rapidly quenched Pd thin films. Crystal nucleation and growth rates are determined over the temperature range $700$--$1150~\mathrm{K}$ ($0.38$--$0.65 T_{\mathrm{m}}$) by analysing the evolution of the microstructure during the liquid-to-crystal transition. The self-diffusion coefficient of Pd, obtained from the atomic mean-squared displacement, follows Arrhenius behaviour over the investigated temperature range, with an activation energy of $467(6)~\mathrm{meV/atom}$, consistent with available data for supercooled liquid metals. The steady-state homogeneous nucleation rate exhibits a maximum of approximately $4 \times 10^{35}~\mathrm{m^{-3} s^{-1}}$ near $0.5 T_{\mathrm{m}}$. Crystal growth occurs at velocities of the order of metres per second, with a temperature dependence consistent with diffusion-limited Wilson-Frenkel kinetics rather than the collision-limited regime. Based on multiple statistically independent simulations, a time-temperature-transformation (TTT) diagram for crystallisation onset is constructed. The TTT curve exhibits a nose near $0.5 T_{\mathrm{m}}$ and $100~\mathrm{ps}$, corresponding to a critical cooling rate for vitrification on the order of $10^{13}~\mathrm{K s^{-1}}.$ The simulations reproduce the crystallisation onset time and temperature observed in time-resolved X-ray diffraction experiments on optically molten Pd thin films quenched at $5 \times 10^{11}~\mathrm{K s^{-1}}.$ These results indicate that homogeneous, rather than heterogeneous, nucleation governs the achievable supercooling in the experimentally studied films.

cond-mat.mtrl-sci↗

arXiv2025

Fluorescence intensity correlations enable 3D imaging without sample rotations

Lensless X-ray imaging provides element-specific nanoscale insights into thick samples beyond the reach of conventional light and electron microscopy. Coherent diffraction imaging (CDI) methods, such as ptychographic tomography, can recover three-dimensional (3D) nanoscale structures but require extensive sample rotation, adding complexity to experiments. X-ray elastic-scattering patterns from a single sample orientation are highly directional and provide limited 3D information about the structure. In contrast to X-ray elastic scattering, X-ray fluorescence is emitted mostly isotropically. However, first-order spatial coherence has traditionally limited nanoscale fluorescence imaging to single-crystalline samples. Here, we demonstrate that intensity correlations of X-ray fluorescence excited by ultrashort X-ray pulses contain 3D structural information of non-periodic, stationary objects. In our experiment, we illuminated a vanadium foil within a sub-200 nm X-ray laser beam focus. Without changing the sample orientation, we recorded 16 distinct specimen projections using detector regions covering different photon incidence angles relative to the X-ray free-electron laser (FEL) beam. The projections varied systematically as the fluorescing volume was translated along an astigmatism, confirming that FEL-induced fluorescence reflects real-space structural changes. Our results establish a new approach for lensless 3D imaging of non-periodic specimens using fluorescence intensity correlations, with broad implications for materials science, chemistry, and nanotechnology.

physics.optics↗

arXiv2025

A low-background setup for in-situ X-ray total scattering combined with fast scanning calorimetry

We demonstrate a setup combining fast scanning calorimetry with X-ray total scattering at a synchrotron beamline, allowing for \emph{in-situ} characterizations of the nano-scale structure of samples during and after temperature scans. The setup features a portable vacuum chamber giving high signal-to-background ratio even on amorphous samples, which enables the observation of detailed structural changes between different sample states. We show three use cases, including one which leverages the high cooling rate of 10$^4$\,K/s achievable by this setup. Our demonstration opens the door to various applications in materials science where it is important to understand the interplay between structure and thermodynamics.

physics.ins-det↗

arXiv2024

Dynamics of Nanoscale Phase Decomposition in Laser Ablation

Femtosecond laser ablation is a process that bears both fundamental physics interest and has wide industrial applications. For decades, the lack of probes on the relevant time and length scales has prevented access to the highly nonequilibrium phase decomposition processes triggered by laser excitation. Enabled by the unprecedented intense femtosecond X-ray pulses delivered by an X-ray free electron laser, we report here results of time-resolved small angle scattering measurements on the dynamics of nanoscale phase decomposition in thin gold films upon femtosecond laser-induced ablation. By analyzing the features imprinted onto the small angle diffraction patterns, the transient heterogeneous density distributions within the ablation plume as obtained from molecular dynamics simulations get direct experimental confirmation.

cond-mat.mtrl-sci↗

arXiv2023

Hard X-ray Generation and Detection of Nanometer-Scale Localized Coherent Acoustic Wave Packets in SrTiO$_3$ and KTaO$_3$

We demonstrate that the absorption of femtosecond x-ray pulses can excite quasi-spherical high-wavevector coherent acoustic phonon wavepackets using an all x-ray pump and probe scattering experiment. The time- and momentum-resolved diffuse scattering signal is consistent with strain pulses induced by the rapid electron cascade dynamics following photoionization at uncorrelated excitation centers. We quantify key parameters of this process, including the localization size of the strain wavepacket and the energy absorption efficiency, which are determined by the photoelectron and Auger electron cascade dynamics, as well as the electron-phonon interaction. In particular, we obtain the localization size of the observed strain wave packet to be 1.5 and 2.5 nm for bulk SrTiO$_3$ and KTaO$_3$ single crystals, even though there are no nanoscale structures or light-intensity patterns that would ordinarily be required to generate acoustic waves of wavelengths much shorter than the penetration depth. Whereas in GaAs and GaP we do not observe a signal above background. The results provide crucial information on x-ray matter interactions, which sheds light on the mechanism of x-ray energy deposition, and the study of high wavevector acoustic phonons and thermal transport at the nanoscale.

cond-mat.mtrl-sci↗

arXiv2023

Directly observing atomic-scale relaxations of a glass forming liquid using femtosecond X-ray photon correlation spectroscopy

Glass forming liquids exhibit structural relaxation behaviors, reflecting underlying atomic rearrangements on a wide range of timescales. These behaviors play a crucial role in determining many material properties. However, the relaxation processes on the atomic scale are not well understood due to the experimental difficulties in directly characterizing the evolving correlations of atomic order in disordered systems. Here, taking the model system Ge15Te85, we demonstrate an experimental approach that probes the relaxation dynamics by scattering the coherent X-ray pulses with femtosecond duration produced by X-ray free electron lasers (XFELs). By collecting the summed speckle patterns from two rapidly successive, nearly identical X-ray pulses generated using a split-delay system, we can extract the contrast decay of speckle patterns originating from sample dynamics and observe the full decorrelation of local order on the sub-picosecond timescale. This provides the direct atomic-level evidence of fragile liquid behavior of Ge15Te85. Our results demonstrate the strategy for XFEL-based X-ray photon correlation spectroscopy (XPCS), attaining femtosecond temporal and atomic-scale spatial resolutions. This twelve orders of magnitude extension from the millisecond regime of synchrotron-based XPCS opens a new avenue of experimental studies of relaxation dynamics in liquids, glasses, and other highly disordered systems.

cond-mat.mtrl-sci↗

arXiv2023

Speed of sound in methane under conditions of planetary interiors

We present direct observations of acoustic waves in warm dense matter. We analyze wave-number- and energy-resolved x-ray spectra taken from warm dense methane created by laser heating a cryogenic liquid jet. X-ray diffraction and inelastic free-electron scattering yield sample conditions of 0.3$\pm$0.1 eV and 0.8$\pm$0.1 g/cm$^3$, corresponding to a pressure of $\sim$13 GPa. Inelastic x-ray scattering was used to observe the collective oscillations of the ions. With a highly improved energy resolution of $\sim$50 meV, we could clearly distinguish the Brillouin peaks from the quasielastic Rayleigh feature. Data at different wave numbers were utilized to derive a sound speed of 5.9$\pm$0.5 km/s, marking a high-temperature data point for methane and demonstrating consistency with Birch's law in this parameter regime.

physics.plasm-ph↗

arXiv2023

Structural pathways for ultrafast melting of optically excited thin polycrystalline Palladium films

Due to its extremely short timescale, the non-equilibrium melting of metals is exceptionally difficult to probe experimentally. The knowledge of melting mechanisms is thus based mainly on the results of theoretical predictions. This work reports on the investigation of ultrafast melting of thin polycrystalline Pd films studied by optical laser pump - X-ray free-electron laser probe experiments and molecular-dynamics simulations. By acquiring X-ray diffraction snapshots with sub-picosecond resolution, we capture the sample's atomic structure during its transition from the crystalline to the liquid state. Bridging the timescales of experiments and simulations allows us to formulate a realistic microscopic picture of melting. We demonstrate that the existing models of strongly non-equilibrium melting, developed for systems with relatively weak electron-phonon coupling, remain valid even for ultrafast heating rates achieved in femtosecond laser-excited Pd. Furthermore, we highlight the role of pre-existing and transiently generated crystal defects in the transition to the liquid state.

cond-mat.mtrl-sci↗

arXiv2022

Structural changes across thermodynamic maxima in supercooled liquid tellurium: a water-like scenario

Liquid polymorphism is an intriguing phenomenon which has been found in a few single-component systems, the most famous being water. By supercooling liquid Te to more than 130 K below its melting point and performing simultaneous small-angle and wide-angle X-ray scattering measurements, we observe clear maxima in its thermodynamic response functions around 615 K, suggesting the possible existence of liquid polymorphism. A close look at the underlying structural evolution shows the development of intermediate-range order upon cooling, most strongly around the thermodynamic maxima, which we attribute to bond-orientational ordering. The striking similarities between our results and those of water, despite the lack of hydrogen-bonding and tetrahedrality in tellurium, indicate that water-like anomalies may be a general phenomenon among liquid systems with competing bond- and density-ordering.

cond-mat.soft↗

arXiv2022

Generation of highly mutually coherent hard x-ray pulse pairs with an amplitude-splitting delay line

Beam splitters and delay lines are among the key building blocks of modern-day optical laser technologies. Progress in x-ray free electron laser source development and applications over the past decade is calling for their counter part operating in the Angstrom wavelength regime. Recent efforts in x-ray optics development have demonstrated relatively stable delay lines that most often adopted the division of wavefront approach for the beam splitting and recombination configuration. However, the two recombined beams have yet to achieve sufficient mutual coherence to enable applications such as interferometry, correlation spectroscopy, and nonlinear spectroscopy. We present the first experimental realization of the generation of highly mutually coherent pulse pairs using an amplitude-split delay line design based on transmission grating beam splitters and channel-cut crystal optic delay lines. The performance of the prototype system was analyzed in the context of x-ray coherent scattering and correlation spectroscopy, where we obtained nearly identical high-contrast speckle patterns from both branches. We show in addition the high level of dynamical stability during continuous delay scans, a capability essential for high sensitivity ultra-fast measurements.

physics.optics↗

arXiv2021

Universal two-component dynamics in supercritical fluids

Despite the technological importance of supercritical fluids, controversy remains about the details of their microscopic dynamics. In this work, we study four supercritical fluid systems -- water, Si, Te, and Lennard-Jones fluid -- \emph{via} classical molecular dynamics simulations. A universal two-component behavior is observed in the intermolecular dynamics of these systems, and the changing ratio between the two components leads to a crossover from liquidlike to gaslike dynamics, most rapidly around the Widom line. We find evidence to connect the liquidlike component dominating at lower temperatures with intermolecular bonding, and the component prominent at higher temperatures with free-particle, gaslike dynamics. The ratio between the components can be used to describe important properties of the fluid, such as its self-diffusion coefficient, in the transition region. Our results provide insight into the fundamental mechanism controlling the dynamics of supercritical fluids, and highlight the role of spatiotemporally inhomogenous dynamics even in thermodynamic states where no large-scale fluctuations exist in the fluid.

cond-mat.soft↗

arXiv2020

Two-component dynamics and the liquid-like to gas-like crossover in supercritical water

Molecular-scale dynamics in sub- to super-critical water is studied with inelastic X-ray scattering and molecular dynamics simulations. The obtained longitudinal current correlation spectra can be decomposed into two main components: a low-frequency (LF), gas-like component and a high-frequency (HF) component arising from the O--O stretching mode between hydrogen-bonded molecules, reminiscent of the longitudinal acoustic mode in ambient water. With increasing temperature, the hydrogen-bond network diminishes and the spectral weight shifts from HF to LF, leading to a transition from liquid-like to gas-like dynamics with rapid changes around the Widom line.

cond-mat.soft↗

arXiv2015

A New Technique for Large-Area Detection of High Energy Particles using Ultra-Fast Magnetic Sensing

Cascades from high-energy particles produce a brief current and associated magnetic fields. Even sub-nanosecond duration magnetic fields can be detected with a relatively low bandwidth system by latching image currents on a capacitor. At accelerators, this technique is employed routinely by beam-current monitors, which work for pulses even as fast as femtoseconds. We discuss scaling up these instruments in size, to 100 meters and beyond, to serve as a new kind of ground- and space-based high-energy particle detector which can instrument large areas relatively inexpensively. This new technique may be used to detect and/or veto ultra-high energy cosmic-ray showers above 100 PeV. It may also be applied to searches for hypothetical highly charged particles. In addition, these detectors may serve to search for extremely short magnetic field pulses of any origin, faster than other detectors by orders of magnitude.

physics.ins-det↗