arXiv subjects

Sanghoon Song

Publications and source records attributed to Sanghoon Song.

18 recordsLinked to original sources

arXiv2026

Broadband hard X-ray attosecond pulses from extremely chirped electron beams

Attosecond pulses from free-electron lasers have opened the doors to atomic site-specific studies of bound electronic dynamics on their natural, sub-femtosecond timescales. Key to their success has been electron beam shaping techniques enabling the generation of sub-femtosecond current spikes with peak currents on the order of 10 kA. We demonstrate in an RF linac the generation of current spikes with extreme chirps on the order of 350 MeV/micron, directly competitive with the chirps expected from beam-driven plasma wakefield accelerators. Leveraging chirp-taper compensation, we use these highly chirped beams to generate hard X-ray attosecond pulses with bandwidths exceeding 30 eV, a factor of two beyond previous demonstrations. We simultaneously present the first explicit experimental evidence of chirp-taper compensation in an attosecond XFEL, finding that optimal tapering improves the bandwidth and pulse energy by factors of two and five, respectively, for our conditions. In addition to the immediate utility of such broadband hard X-ray pulses, electron beams with such extreme chirps can be utilized for unique new experimental modalities by performing further compression after the undulators. Such post-lasing compression can enable subsequent superradiant light emission at longer wavelengths, or direct excitation of quantum systems with the beam's intense space-charge field for unique attosecond pump-probe possibilities.

physics.acc-ph↗

arXiv2025

Data Driven Drift Correction For Complex Optical Systems

To exploit the thousand-fold increase in spectral brightness of modern light sources, increasingly intricate experiments are being conducted that demand extremely precise beam trajectory. Maintaining the optimal trajectory over several hours of an experiment with the needed precision necessitates active drift control. Here, we outline Time-Varying Bayesian Optimization (TVBO) as a data driven approach for robust drift correction, and illustrate its application for a split and delay optical system composed of six crystals and twelve input dimensions. Using numerical simulations, we exhibit the application of TVBO for linear drift, non-smooth temporal drift as well as constrained TVBO for multi-objective control settings, representing real-life operating conditions. This approach can be easily adapted to other X-ray beam conditioning and guidance systems, including multi-crystal monochromators and grazing-incidence mirrors, to maintain sub-micron and nanoradian beam stability over the course of an experiment spanning several hours.

physics.optics↗

arXiv2025

Nanoscale Ultrafast Lattice Modulation with Hard X-ray Free Electron Laser

Understanding and controlling microscopic dynamics across spatial and temporal scales has driven major progress in science and technology over the past several decades. While ultrafast laser-based techniques have enabled probing nanoscale dynamics at their intrinsic temporal scales down to femto- and attoseconds, the long wavelengths of optical lasers have prevented the interrogation and manipulation of such dynamics with nanoscale spatial specificity. With advances in hard X-ray free electron lasers (FELs), significant progress has been made developing X-ray transient grating (XTG) spectroscopy, aiming at the coherent control of elementary excitations with nanoscale X-ray standing waves. So far, XTGs have been probed only at optical wavelengths, thus intrinsically limiting the achievable periodicities to several hundreds of nm. By achieving sub-femtosecond synchronization of two hard X-ray pulses at a controlled crossing angle, we demonstrate the generation of an XTG with spatial periods of 10 nm. The XTG excitation drives a thermal grating that drives coherent monochromatic longitudinal acoustic phonons in the cubic perovskite, SrTiO3 (STO). With a third X-ray pulse with the same photon energy, time-and-momentum resolved measurement of the XTG-induced scattering intensity modulation provides evidence of ballistic thermal transport at nanometer scale in STO. These results highlight the great potential of XTG for studying high-wave-vector excitations and nanoscale transport in condensed matter, and establish XTG as a powerful platform for the coherent control and study of nanoscale dynamics.

physics.optics↗

arXiv2025

Terahertz-field activation of polar skyrons

Unraveling collective modes arising from coupled degrees of freedom is crucial for understanding complex interactions in solids and developing new functionalities. Unique collective behaviors emerge when two degrees of freedom, ordered on distinct length scales, interact. Polar skyrmions, three-dimensional electric polarization textures in ferroelectric superlattices, disrupt the lattice continuity at the nanometer scale with nontrivial topology, leading to previously unexplored collective modes. Here, using terahertz-field excitation and femtosecond x-ray diffraction, we discovered subterahertz collective modes, dubbed 'skyrons', which appear as swirling patterns of atomic displacements functioning as atomic-scale gearsets. Momentum-resolved time-domain measurements of diffuse scattering revealed an avoided crossing in the dispersion relation of skyrons. We further demonstrated that the amplitude and dispersion of skyrons can be controlled by sample temperature and electric-field bias. Atomistic simulations and dynamical phase-field modeling provided microscopic insights into the three-dimensional crystallographic and polarization dynamics. The discovery of skyrons and their coupling with terahertz fields opens avenues for ultrafast control of topological polar structures.

cond-mat.mtrl-sci↗

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↗

arXiv2024

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↗

arXiv2024

In situ coherent X-ray scattering reveals polycrystalline structure and discrete annealing events in strongly-coupled nanocrystal superlattices

Solution-phase bottom up self-assembly of nanocrystals into superstructures such as ordered superlattices is an attractive strategy to generate functional materials of increasing complexity, including very recent advances that incorporate strong interparticle electronic coupling. While the self-assembly kinetics in these systems have been elucidated and related to the product characteristics, the weak interparticle bonding interactions suggest the superstructures formed could continue to order within the solution long after the primary nucleation and growth have occurred, even though the mechanism of annealing remains to be elucidated. Here, we use a combination of Bragg coherent diffractive imaging and X-ray photon correlation spectroscopy to create real-space maps of supercrystalline order along with a real-time view of the strain fluctuations in aging strongly coupled nanocrystal superlattices while they remain suspended and immobilized in solution. By combining the results, we deduce that the self-assembled superstructures are polycrystalline, initially comprising multiple nucleation sites, and that shear avalanches at grain boundaries continue to increase crystallinity long after growth has substantially slowed. This multimodal approach should be generalizable to characterize a breadth of materials in situ in their native chemical environments, thus extending the reach of high-resolution coherent X-ray characterization to the benefit of a much wider range of physical systems.

cond-mat.mtrl-sci↗

arXiv2024

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↗

arXiv2022

Ultrafast x-ray scattering reveals composite amplitude collective mode in the Weyl charge density wave material (TaSe$_4$)$_2$I

We report ultrafast x-ray scattering experiments of the quasi-1D charge density wave (CDW) material (TaSe$_4$)$_2$I following photoexcitation with femtosecond infrared laser pulses. From the time-dependent diffraction signal at the CDW sidebands we identify an amplitude mode derived primarily from the transverse acoustic component of the CDW static distortion. The dynamics of this acoustic amplitude mode are described well by a model of a displacive excitation, which we interpret as mediated through a coupling to the optical phonon component associated with the tetramerization of the Ta chains.

cond-mat.mtrl-sci↗

arXiv2022

Testing the data framework for an AI algorithm in preparation for high data rate X-ray facilities

The advent of next-generation X-ray free electron lasers will be capable of delivering X-rays at a repetition rate approaching 1 MHz continuously. This will require the development of data systems to handle experiments at these type of facilities, especially for high throughput applications, such as femtosecond X-ray crystallography and X-ray photon fluctuation spectroscopy. Here, we demonstrate a framework which captures single shot X-ray data at the LCLS and implements a machine-learning algorithm to automatically extract the contrast parameter from the collected data. We measure the time required to return the results and assess the feasibility of using this framework at high data volume. We use this experiment to determine the feasibility of solutions for `live' data analysis at the MHz repetition rate.

physics.data-an↗

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

Nanoscale heterogeneous dynamics probed by nanosecond x-ray speckle visibility spectroscopy

We report observations of nanosecond nanometer scale heterogeneous dynamics in a free flowing colloidal jet revealed by ultrafast x-ray speckle visibility spectroscopy. The nanosecond double-bunch mode of the Linac Coherent Light Source free electron laser enabled the production of pairs of femtosecond coherent hard x-ray pulses. By exploring the anisotropic summed speckle visibility which relates to the correlation functions, we are able to evaluate not only the average particle flow rate in a colloidal nanoparticle jet, but also the heterogeneous flow field within. The reported methodology presented here establishes the foundation for the study of nano- and atomic-scale heterogeneous fluctuations in complex matter using x-ray free electron laser sources.

cond-mat.soft↗

arXiv2019

Speckle correlation as a monitor of X-ray free electron laser induced crystal lattice deformation

X-ray free electron lasers (X-FELs) present new opportunities to study ultrafast lattice dynamics in complex materials. While the unprecedented source brilliance enables high fidelity measurement of structural dynamics, it also raises experimental challenges related to the understanding and control of beam-induced irreversible structural changes in samples that can ultimately impact the interpretation of experimental results. This is also important for designing reliable high performance X-ray optical components. In this work, we investigate X-FEL beam-induced lattice alterations by measuring the shot-to-shot evolution of near-Bragg coherent scattering from a single crystalline germanium sample. We show that X-ray photon correlation analysis of sequential speckle patterns measurements can be used to monitor the nature and extent of lattice rearrangements. Abrupt, irreversible changes are observed following intermittent high-fluence monochromatic X-ray pulses, thus revealing the existence of a threshold response to X-FEL pulse intensity.

physics.app-ph↗

arXiv2019

Femtosecond laser produced periodic plasma in a colloidal crystal probed by XFEL radiation

With the rapid development of short-pulse intense laser sources, studies of matter under extreme irradiation conditions enter further unexplored regimes. In addition, an application of X-ray Free- Electron Lasers (XFELs), delivering intense femtosecond X-ray pulses allows to investigate sample evolution in IR pump - X-ray probe experiments with an unprecedented time resolution. Here we present the detailed study of periodic plasma created from the colloidal crystal. Both experimental data and theory modeling show that the periodicity in the sample survives to a large extent the extreme excitation and shock wave propagation inside the colloidal crystal. This feature enables probing the excited crystal, using the powerful Bragg peak analysis, in contrast to the conventional studies of dense plasma created from bulk samples for which probing with Bragg diffraction technique is not possible. X-ray diffraction measurements of excited colloidal crystals may then lead towards a better understanding of matter phase transitions under extreme irradiation conditions.

cond-mat.soft↗

arXiv2018

Anisotropic structural dynamics of monolayer crystals revealed by femtosecond surface x-ray scattering

X-ray scattering is one of the primary tools to determine crystallographic configuration with atomic accuracy. However, the measurement of ultrafast structural dynamics in monolayer crystals remains a long-standing challenge due to a significant reduction of diffraction volume and complexity of data analysis, prohibiting the application of ultrafast x-ray scattering to study nonequilibrium structural properties at the two-dimensional limit. Here, we demonstrate femtosecond surface x-ray diffraction in combination with crystallographic model-refinement calculations to quantify the ultrafast structural dynamics of monolayer WSe$_2$ crystals supported on a substrate. We found the absorbed optical photon energy is preferably coupled to the in-plane lattice vibrations within 2 picoseconds while the out-of-plane lattice vibration amplitude remains unchanged during the first 10 picoseconds. The model-assisted fitting suggests an asymmetric intralayer spacing change upon excitation. The observed nonequilibrium anisotropic structural dynamics in two-dimensional materials agrees with first-principles nonadiabatic modeling in both real and momentum space, marking the distinct structural dynamics of monolayer crystals from their bulk counterparts. The demonstrated methods unlock the benefit of surface sensitive x-ray scattering to quantitatively measure ultrafast structural dynamics in atomically thin materials and across interfaces.

cond-mat.mtrl-sci↗

arXiv2018

The Ultrafast Einstein-De Haas Effect

The original observation of the Einstein-de Haas effect was a landmark experiment in the early history of modern physics that illustrates the relationship between magnetism and angular momentum. Today the effect is still discussed in elementary physics courses to demonstrate that the angular momentum associated with the aligned electron spins in a ferromagnet can be converted to mechanical angular momentum by reversing the direction of magnetisation using an external magnetic field. In recent times, a related problem in magnetism concerns the time-scale over which this angular momentum transfer can occur. It is known experimentally for several metallic ferromagnets that intense photoexcitation leads to a drop in the magnetisation on a time scale shorter than 100 fs, a phenomenon called ultrafast demagnetisation. The microscopic mechanism for this process has been hotly debated, with one key question still unanswered: where does the angular momentum go on these sub-picosecond time scales? Here we show using femtosecond time-resolved x-ray diffraction that a large fraction of the angular momentum lost from the spin system on the laserinduced demagnetisation of ferromagnetic iron is transferred to the lattice on sub-picosecond timescales, manifesting as a transverse strain wave that propagates from the surface into the bulk. By fitting a simple model of the x-ray data to simulations and optical data, we roughly estimate that the angular momentum occurs on a time scale of 200 fs and corresponds to 80% of the angular momentum lost from the spin system. Our results show that interaction with the lattice plays an essential role in the process of ultrafast demagnetisation in this system.

cond-mat.str-el↗

arXiv2015

Watching coherent molecular structural dynamics during photoreaction: beyond kinetic description

A deep understanding of molecular photo-transformations is challenging because of the complex interaction between the configurations of electrons and nuclei. An initial optical excitation dissipates energy into electronic and structural degrees of freedom, often in less than one trillionth (10^-12) of a second. Molecular dynamics induced by photoexcitation have been very successfully studied with femtosecond optical spectroscopies, but electronic and nuclear dynamics are often very difficult to disentangle. X-ray based spectroscopies can reduce the ambiguity between theoretical models and experimental data, but it is only with the recent development of bright ultrafast X-ray sources, that key information during transient molecular processes can be obtained on their intrinsic timescale. In this letter, Free Electron Laser (FEL) radiation is used to measure ultrafast changes in the X-ray Absorption Near Edge Structure (XANES) during the prototypical photoreaction of a spin crossover compound. We reveal its transformation from the ligand-located electronic photoexcitation to the structural trapping of the high spin state. The results require a description beyond a kinetic model and provide a direct observation of a dynamic breathing of the main structural change. The coherent structural oscillations (period of ~265 fs) in the photoproduct potential lose synchrony within ~330 fs, whereas incoherent motions reveal the energy redistribution and vibrational cooling within ~1.6 ps. We foresee that ultrafast X-ray spectroscopies will provide invaluable insight to understand the complex physics of fundamental light induced phenomena, which are of prime interest in a multitude of chemical, physical and biological processes.

physics.chem-ph↗

arXiv2013

Performance of an LPD prototype detector at MHz frame rates under Synchrotron and FEL radiation

A MHz frame rate X-ray area detector (LPD - Large Pixel Detector) is under development by the Rutherford Appleton Laboratory for the European XFEL. The detector will have 1 million pixels and allows analogue storage of 512 images taken at 4.5 MHz in the detector front end. The LPD detector has 500 mm thick silicon sensor tiles that are bump bonded to a readout ASIC. The ASICs preamplifier provides relatively low noise at high speed which results in a high dynamic range of 10^5 photons over an energy range of 5-20 keV. Small scale prototypes of 32x256 pixels (LPD 2-Tile detector) and 256x256 pixels (LPD supermodule detector) are now available for X-ray tests. The performance of prototypes of the detector is reported for first tests under synchrotron radiation (PETRA III at DESY) and Free-Electron-Laser radiation (LCLS at SLAC). The initial performance of the detector in terms of signal range and noise, radiation hardness and spatial and temporal response are reported. The main result is that the 4.5 MHz sampling detection chain is reliably working, including the analogue on-chip memory concept. The detector is at least radiation hard up to 5 MGy at 12 keV. In addition the multiple gain concept has been demonstrated over a dynamic range to 10^4 at 12 keV with a readout noise equivalent to <1 photon rms in its most sensitive mode.

physics.ins-det↗