X-ray Free-electron Laser Pulses Research Articles

Sub-photon accuracy noise reduction of a single shot coherent diffraction pattern with an atomic model trained autoencoder

Single-shot imaging with femtosecond X-ray lasers is a powerful measurement technique that can achieve both high spatial and temporal resolution. However, its accuracy has been severely limited by the difficulty of applying conventional noise-reduction processing. This study uses deep learning to validate noise reduction techniques, with autoencoders serving as the learning model. Focusing on the diffraction patterns of nanoparticles, we simulated a large dataset treating the nanoparticles as composed of many independent atoms. Three neural network architectures are investigated: neural network, convolutional neural network and U-net, with U-net showing superior performance in noise reduction and subphoton reproduction. We also extended our models to apply to diffraction patterns of particle shapes different from those in the simulated data. We then applied the U-net model to a coherent diffractive imaging study, wherein a nanoparticle in a microfluidic device is exposed to a single X-ray free-electron laser pulse. After noise reduction, the reconstructed nanoparticle image improved significantly even though the nanoparticle shape was different from the training data, highlighting the importance of transfer learning.

A workflow for single-particle structure determination via iterative phasing of rotational invariants in fluctuation X-ray scattering.

Fluctuation X-ray scattering (FXS) offers a complementary approach for nano- and bioparticle imaging with an X-ray free-electron laser (XFEL), by extracting structural information from correlations in scattered XFEL pulses. Here a workflow is presented for single-particle structure determination using FXS. The workflow includes procedures for extracting the rotational invariants from FXS patterns, performing structure reconstructions via iterative phasing of the invariants, and aligning and averaging multiple reconstructions. The reconstruction pipeline is implemented in the open-source software xFrame and its functionality is demonstrated on several simulated structures.

Extreme focusing of hard X-ray free-electron laser pulses enables 7 nm focus width and 1022 W cm−2 intensity

Extreme focusing of hard X-ray free-electron laser pulses enables 7 nm focus width and 1022 W cm−2 intensity

Thermoelastic effects in Bragg reflectors as a potential bottleneck for XFELs with megahertz repetition rate

Bragg reflectors are essential for beam transport in X-ray free-electron laser (XFEL) facilities. On interaction with Bragg reflectors, a part of the pulse energy will be absorbed, causing the propagation of displacement waves due to rapid thermal expansion. It is suspected that these waves may cause stability problems for XFELs operating with megahertz repetition rates. Here, we experimentally investigate the displacement of a diamond Bragg reflector induced by an optical ultra-violet laser pulse, simulating XFEL pulses with mJ pulse energy, both at room temperature and cryogenic temperatures. Our experiment shows negligible damping of the displacement waves on µs timescales, which could cause disruption for subsequent XFEL pulses. We compare our measurements to a simulation framework based on the assumptions of local thermodynamic equilibrium and classical mechanics, observing reasonable agreement. Our results show that thermoelastic effects are critical for a reliable stability assessment of Bragg reflectors, but are often overlooked.

Transient X-Ray Absorption Near Edge Structure Spectroscopy Using Broadband Free-Electron Laser Pulses.

A new method for time-resolved X-ray absorption near edge structure (XANES) spectroscopy that enables faster data acquisition and requires smaller sample quantities for high-quality data, thus allowing the analysis of more samples in a shorter time is introduced. The method uses large bandwidth free electron laser pulses to measure laser-excited XANES spectra in transmission mode. A beam-splitting grating configuration allows simultaneous measurements of the spectra of the incoming X-ray Free Electron Laser (XFEL) pulses and transmission XANES, which is crucial for compensating the pulse-dependent intensity and spectrum fluctuations due to the self-amplified spontaneous emission operation. The implementation of this new methodology is applied on a liquid solution of ammonium iron(III) oxalate jet and is compared to previous results, showing great improvements in the speed of acquisition and spectral resolution, and the ability to measure a large 2-D spectral-time map quickly.

The collapse of a sonoluminescent cavitation bubble imaged with X-ray free-electron laser pulses

Single bubble sonoluminescence (SBSL) is the phenomenon of synchronous light emission due to the violent collapse of a single spherical bubble in a liquid, driven by an ultrasonic field. During the bubble collapse, matter inside the bubble reaches extreme conditions of several gigapascals and temperatures on the order of 10000 K, leading to picosecond flashes of visible light. To this day, details regarding the energy focusing mechanism rely on simulations due to the fast dynamics of the bubble collapse and spatial scales below the optical resolution limit. In this work we present phase-contrast holographic imaging with single x-ray free-electron laser (XFEL) pulses of a SBSL cavitation bubble in water. X-rays probe the electron density structure and by that provide a uniquely new view on the bubble interior and its collapse dynamics. The involved fast time-scales are accessed by sub-100 fs XFEL pulses and a custom synchronization scheme for the bubble oscillator. We find that during the whole oscillation cycle the bubble’s density profile can be well described by a simple step-like structure, with the radius R following the dynamics of the Gilmore model. The quantitatively measured internal density and width of the boundary layer exhibit a large variance. Smallest reconstructed bubble sizes reach down to R≃0.8μm , and are consistent with spherical symmetry. While we here achieved a spatial resolution of a few 100 nm, the visibility of the bubble and its internal structure is limited by the total x-ray phase shift which can be scaled with experimental parameters.

High-energy-resolution off-resonant spectroscopy with self-seeded x-ray free-electron laser pulses.

This paper presents the implementation of high-energy-resolution off-resonant spectroscopy (HEROS) measurements using self-seeded x-ray free-electron laser (XFEL) pulses. This study systematically investigated XFEL conditions, including photon energy and accumulated shot numbers, to optimize the measurement efficiency for copper foil samples near the K-edge. The x-ray absorption spectra reconstructed using HEROS were compared with those derived from fluorescence-yield measurements. The HEROS-based spectra exhibited consistent line shapes independent of the sample thickness. The potential application of HEROS to high-temperature copper was also explored. HEROS offers distinct advantages including scan-free measurement of x-ray absorption spectra with reduced core-hole lifetime broadening and self-absorption effects. Using self-seeded XFEL pulses, HEROS facilitates single-shot-based pump-probe measurements to investigate the ultrafast dynamics in various materials and diverse conditions.

Comprehensive Application of XFEL Microcrystallography for Challenging Targets in Various Organic Compounds.

There is a growing demand for structure determination from small crystals, and the three-dimensional electron diffraction (3D ED) technique can be employed for this purpose. However, 3D ED has certain limitations related to the crystal thickness and data quality. We here present the application of serial X-ray crystallography (SX) with X-ray free electron lasers (XFELs) to small (a few μm or less) and thin (a few hundred nm or less) crystals of novel compounds dispersed on a substrate. For XFEL exposures, two-dimensional (2D) scanning of the substrate coupled with rotation enables highly efficient data collection. The recorded patterns can be successfully indexed using lattice parameters obtained through 3D ED. This approach is especially effective for challenging targets, including pharmaceuticals and organic materials that form preferentially oriented flat crystals in low-symmetry space groups. Some of these crystals have been difficult to solve or have yielded incomplete solutions using 3D ED. Our extensive analyses confirmed the superior quality of the SX data regardless of crystal orientations. Additionally, 2D scanning with XFEL pulses gives an overall distribution of the samples on the substrate, which can be useful for evaluating the properties of crystal grains and the quality of layered crystals. Therefore, this study demonstrates that XFEL crystallography has become a powerful tool for conducting structure studies of small crystals of organic compounds.

3D atomic structure from a single X-ray free electron laser pulse

X-ray Free Electron Lasers (XFEL) are cutting-edge pulsed x-ray sources, whose extraordinary pulse parameters promise to unlock unique applications. Several new methods have been developed at XFELs; however, no methods are known, which allow ab initio atomic level structure determination using only a single XFEL pulse. Here, we present experimental results, demonstrating the determination of the 3D atomic structure from data obtained during a single 25 fs XFEL pulse. Parallel measurement of hundreds of Bragg reflections was done by collecting Kossel line patterns of GaAs and GaP. To the best of our knowledge with these measurements, we reached the ultimate temporal limit of the x-ray structure solution possible today. These measurements open the way for obtaining crystalline structures during non-repeatable fast processes, such as structural transformations. For example, the atomic structure of matter at extremely non-ambient conditions or transient structures formed in irreversible physical, chemical, or biological processes may be captured in a single shot measurement during the transformation. It would also facilitate time resolved pump-probe structural studies making them significantly shorter than traditional serial crystallography.

FURION: modeling of FEL pulses propagation in dispersive soft X-ray beamline systems.

Modern X-ray free-electron lasers (XFELs) can generate pulses with durations ranging from femtoseconds to attoseconds. The numerical evaluation of ultra-short XFEL pulses through beamline systems is a critical process of beamline system design. However, the bandwidth of such ultra-short XFEL pulses is often non-negligible, and the propagation cannot be simply approximated using the central wavelength, especially in dispersive beamline systems. We developed a numerical model which is called Fourier optics based Ultrashort x-Ray pulse propagatION tool (FURION). This model can not only be used to simulate dispersive beamline systems but also to evaluate non-dispersive beamline systems. The FURION model utilizes Fresnel integral and angular spectrum integral to perform ultra-short XFEL pulse propagation in free space. We also present the method for XFEL pulse propagation through different types of dispersive gratings, which are commonly used in soft X-ray beamline systems. By using FURION, a start-to-end simulation of the FEL-1 beamline system at Shenzhen superconducting soft X-ray free electron laser (S3FEL) is carried out. This model can also be used to evaluate gratings-based spectrometers, beam splitters, pulse compressors, and pulse stretchers. This work provides valuable insights into the start-to-end simulation of X-ray beamline systems.

Characterization of Biological Samples Using Ultra-Short and Ultra-Bright XFEL Pulses.

The advent of X-ray Free Electron Lasers (XFELs) has ushered in a transformative era in the field of structural biology, materials science, and ultrafast physics. These state-of-the-art facilities generate ultra-bright, femtosecond-long X-ray pulses, allowing researchers to delve into the structure and dynamics of molecular systems with unprecedented temporal and spatial resolutions. The unique properties of XFEL pulses have opened new avenues for scientific exploration that were previously considered unattainable. One of the most notable applications of XFELs is in structural biology. Traditional X-ray crystallography, while instrumental in determining the structures of countless biomolecules, often requires large, high-quality crystals and may not capture highly transient states of proteins. XFELs, with their ability to produce diffraction patterns from nanocrystals or even single particles, have provided solutions to these challenges. XFEL has expanded the toolbox of structural biologists by enabling structural determination approaches such as Single Particle Imaging (SPI) and Serial X-ray Crystallography (SFX). Despite their remarkable capabilities, the journey of XFELs is still in its nascent stages, with ongoing advancements aimed at improving their coherence, pulse duration, and wavelength tunability.

Protocol using similarity score and improved shrink-wrap algorithm for better convergence of phase-retrieval calculation in X-ray diffraction imaging.

In X-ray diffraction imaging (XDI), electron density maps of a targeted particle are reconstructed computationally from the diffraction pattern alone using phase-retrieval (PR) algorithms. However, the PR calculations sometimes fail to yield realistic electron density maps that approximate the structure of the particle. This occurs due to the absence of structure amplitudes at and near the zero-scattering angle and the presence of Poisson noise in weak diffraction patterns. Consequently, the PR calculation becomes a bottleneck for XDI structure analyses. Here, a protocol to efficiently yield realistic maps is proposed. The protocol is based on the empirical observation that realistic maps tend to yield low similarity scores, as suggested in our prior study [Sekiguchi etal.(2017), J. Synchrotron Rad. 24, 1024-1038]. Among independently and concurrently executed PR calculations, the protocol modifies all maps using the electron-density maps exhibiting low similarity scores. This approach, along with a new protocol for estimating particle shape, improved the probability of obtaining realistic maps for diffraction patterns from various aggregates of colloidal gold particles, as compared with PR calculations performed without the protocol. Consequently, the protocol has the potential to reduce computational costs in PR calculations and enable efficient XDI structure analysis of non-crystalline particles using synchrotron X-rays and X-ray free-electron laser pulses.

Study of population dynamics toward the development of atomic X-ray lasers in the 3–5 keV photon energies

X-ray free-electron lasers (XFELs) are powerful tools for characterizing and probing the properties of matter at atomic resolution on the ultrafast timescale. However, they have certain limitations such as spectral fluctuation and poor temporal coherence. Atomic X-ray lasers offer the narrow bandwidth, longitudinal coherence, and spectral stability that can overcome these limitations. In this paper, we study the interaction of inner-shell vacancy states with high-intensity XFEL pulses. We show that it is possible to achieve population inversion between K-shell and L-shell vacancy states in calcium and titanium when pumped by high-intensity XFEL pulses. These states can be used to generate atomic X-ray laser emission in the 3–5 keV photon energy range.

Self-Referenced Spectral Interferometry for Single-Shot Characterization of Ultrashort Free-Electron Laser Pulses.

An attosecond x-ray pulse with known spectrotemporal information is an essential tool for the investigation of ultrafast electron dynamics in quantum systems. Ultrafast free-electron lasers (FELs) have the unique advantage on unprecedented high intensity at x-ray wavelengths. However, no suitable method has been established so far for the spectrotemporal characterization of these ultrashort x-ray pulses. In this Letter, a simple method has been proposed based on self-referenced spectral interferometry for reconstructing the temporal profile and phase of ultrashort FEL pulses. We have demonstrated that the proposed method is reliable to completely characterize the attosecond x-ray FEL pulses with an error at the level of a few percent. Moreover, the first proof-of-principle experiment has been performed to achieve the single-shot spectrotemporal characterization of ultrashort pulses from a high-gain FEL. The precision of the proposed method will be enhanced with the decrease of the pulse duration, paving a new way for complete attosecond pulse characterization at x-ray FELs.

Coherent sub-femtosecond soft x-ray free-electron laser pulses with nonlinear compression

We demonstrate the generation of coherent soft x-ray free-electron laser (FEL) pulses with a duration below 1 fs using nonlinear compression with a low-charge electron beam (10 pC). The approach is simple, and it does not require any special hardware, so it can be readily implemented at any x-ray FEL facility. We present temporal and spectral diagnostics confirming the production of single-spike sub-femtosecond pulses for photon energies of 642 and 1111 eV. Our work will be important for ultrafast FEL applications requiring soft x-rays.

Spectral-brightness optimization of an X-ray free-electron laser by machine-learning-based tuning.

A machine-learning-based beam optimizer has been implemented to maximize the spectral brightness of the X-ray free-electron laser (XFEL) pulses of SACLA. A new high-resolution single-shot inline spectrometer capable of resolving features of the order of a few electronvolts was employed to measure and evaluate XFEL pulse spectra. Compared with a simple pulse-energy-based optimization, the spectral width was narrowed by half and the spectral brightness was improved by a factor of 1.7. The optimizer significantly contributes to efficient machine tuning and improvement of XFEL performance at SACLA.

Probing shock dynamics inside micro-wire targets after high-intensity laser irradiation using small angle x-ray scattering of a free-electron laser

In this paper, we present an experiment that explores the plasma dynamics of a diameter carbon wire after being irradiated with a near-relativistic-intensity short pulse laser. Using an x-ray free electron laser pulse to measure the small angle x-ray scattering signal, we observe that the scattering surface is bent and prone to instability over tens of picoseconds. The dynamics of this process are consistent with the presence of a sharp, propagating shock front inside the wire, moving at a speed close to the hole boring velocity or that expected from a thermal shock at a few tens of Mbar.

Development of spinning-disk solid sample delivery system for high-repetition rate x-ray free electron laser experiments.

X-ray free-electron lasers (XFELs) deliver intense x-ray pulses that destroy the sample in a single shot by a Coulomb explosion. Experiments using XFEL pulse trains or the new generation of high-repetition rate XFELs require rapid sample replacement beyond those provided by the systems now used at low repletion-rate XFELs. We describe the development and characterization of a system based on a spinning disk to continuously deliver a solid sample into an XFEL interaction point at very high speeds. We tested our system at the Linac Coherent Light Source and European XFEL hard x-ray nano-focus instruments, employing it to deliver a 25 μm copper foil sample, which can be used as a gain medium for stimulated x-ray emission for the proposed x-ray laser oscillator.

Spatiotemporal response of concave VLS grating to ultra-short X-ray pulses.

In soft X-ray free-electron laser (FEL) beamlines, variable-line-spacing (VLS) gratings are often used as dispersive components of monochromators and spectrometers due to their combined dispersion and focusing properties. X-ray FEL pulses passing through the VLS grating can result in not only transverse focusing but also spatiotemporal coupling effects, such as pulse front tilt, pulse front rotation, and pulse stretching. In this paper, we present a theoretical study of the spatiotemporal response of concave VLS gratings to ultra-short X-ray pulses. The theoretical analysis indicates that the tilt angle of the non-zero diffraction orders varies with the propagation distance, and disappears at the focus, where the focal lengths and pulse stretching differ for different diffraction orders. The model demonstrates the pulse duration after the concave VLS grating is the convolution of the initial pulse duration and the stretching term induced by dispersion, while the beam size at the focus in x dimension is the convolution of the geometric scaling beam size and the dispersion term. This work provides a mathematical explanation for the spatiotemporal response of concave VLS grating to ultra-short X-ray pulses and offers valuable insights into the design of FEL grating monochromators, spectrometers, pulse compressors, and pulse stretchers.

Generation of time-synchronized two-color X-ray free-electron laser pulses using phase shifters

To optimize the intensity of X-ray free-electron lasers (XFELs), phase shifters, oriented in phase with the phases of the XFEL pulse and electron beam, are typically installed at undulator lines. Although a π-offset between the phases (i.e., an “out-of-phase” configuration) can suppress the XFEL intensity at resonant frequencies, it can also generate a side-band spectrum, which results in a two-color XFEL pulse; the dynamics of such a pulse can be described using the spontaneous radiation or low gain theory. This attributes of this two-color XFEL pulse can be amplified (log-scale amplification) through an undulator line with out-of-phase phase shifters. In this study, the features of two-color XFEL pulses were evaluated through theory, simulations and experiments performed at Pohang Accelerator Laboratory X-ray Free Electron Laser. The XFEL gain slope and energy separation between the two-color spectral peaks were consistent through theoretical expectation, and the results of simulation and experiment. The experimentally determined two-color XFEL pulse energy was 250 μJ at a photon energy of 12.38 keV with a separation of 60 eV.