Intense X-ray Free-electron Laser Research Articles

Electron-cloud alignment dynamics induced by an intense X-ray free-electron laser pulse: a case study on atomic argon

In an intense X-ray free-electron laser (XFEL) pulse, atoms are sequentially ionised by multiple X-ray photons. Photoionisation generally induces an alignment of the electron cloud of the produced atomic ion regarding its orbital-angular-momentum projections. However, how the alignment evolves during sequential X-ray multi-photon ionisation accompanied by decay processes has been unexplored. Here we present a theoretical prediction of the time evolution of the electron-cloud alignment of argon ions induced by XFEL pulses. To this end, we calculate state-resolved ionisation dynamics of atomic argon interacting with an intense linearly polarised X-ray pulse, which generates ions in a wide range of charge states with non-zero orbital- and spin-angular momenta. Employing time-resolved alignment parameters, we predict the existence of non-trivial alignment dynamics during intense XFEL pulses. This implies that even if initially the atomic electron cloud is perfectly spherically symmetric, X-ray multi-photon ionisation can lead to noticeable reshaping of the electron cloud.

Resonant Raman Auger spectroscopy on transient core-excited Ne ions

Abstract Short-lived core-ionized neon atoms were investigated by measuring under resonant Raman conditions the Auger decay following the excitation of a second core electron into a Rydberg state. Making use of intense and narrow bandwidth x-ray free-electron laser pulses, the photoexcitation spectrum of the femtosecond-lived Ne+1s02s22p6np series was characterized. Energy position and lifetimes of the lower-lying Rydberg states were determined and the final state configurations following the decay of the Ne+1s02s22p63p double-core hole resonance were partially resolved.

Transient absorption of warm dense matter created by an X-ray free-electron laser

Warm dense matter is at the boundary between a plasma and a condensed phase and plays a role in astrophysics, planetary science and inertial confinement fusion research. However, its electronic structure and ionic structure upon irradiation with strong laser pulses remain poorly understood. Here, we use an intense and ultrafast X-ray free-electron laser pulse to simultaneously create and characterize warm dense copper using L-edge X-ray absorption spectroscopy over a large irradiation intensity range. Below a pulse intensity of 1015 W cm−2, an absorption peak below the L edge appears, originating from transient depletion of the 3d band. This peak shifts to lower energy with increasing intensity, indicating the movement of the 3d band upon strong X-ray excitation. At higher intensities, substantial ionization and collisions lead to the transition from reverse saturable absorption to saturable absorption of the X-ray free-electron laser pulse, two nonlinear effects that hold promise for X-ray pulse-shaping. We employ theoretical calculations that combine a model based on kinetic Boltzmann equations with finite-temperature real-space density-functional theory to interpret these observations. The results can be used to benchmark non-equilibrium models of electronic structure in warm dense matter.

X-ray-induced atomic transitions via machine learning: A computational investigation

Intense x-ray free-electron laser pulses can induce multiple sequences of one-photon ionization and accompanying decay processes in atoms, producing highly charged atomic ions. Considering individual quantum states during these processes provides more precise information about the x-ray multiphoton ionization dynamics than the common configuration-based approach. However, in such a state-resolved approach, extremely huge-sized rate-equation calculations are inevitable. Here we present a strategy that embeds machine-learning models into a framework for atomic state-resolved ionization dynamics calculations. Machine learning is employed for the required atomic transition parameters, whose calculations possess the computationally most expensive steps. We find for argon that both feedforward neural networks and random forest regressors can predict these parameters with acceptable, but limited accuracy. State-resolved ionization dynamics of argon, in terms of charge-state distributions and electron and photon spectra, are also presented. Comparing fully calculated and machine-learning-based results, we demonstrate that the proposed machine-learning strategy works in principle and that the performance, in terms of charge-state distributions and electron and photon spectra, is good. Our work establishes a first step toward accelerating the calculation of atomic state-resolved ionization dynamics induced by high-intensity x rays. Published by the American Physical Society 2024

Machine-learning calibration of intense x-ray free-electron-laser pulses using Bayesian optimization

X-ray free-electron lasers (XFELs) have brought new ways to probe and manipulate atomic and molecular dynamics with unprecedented spatial and temporal resolutions. A quantitative comparison of experimental results with their simulated theoretical counterpart, however, generally requires a precise characterization of the spatial and temporal x-ray pulse profile, providing a nonuniform photon distribution. The determination of the pulse profile constitutes a major, yet inevitable, challenge. Here, we propose a calibration scheme for intense XFEL pulses utilizing a set of experimental charge-state distributions of light noble gas atoms at a series of pulse energies in combination with first-principles simulations of the underlying atomic x-ray multiphoton ionization dynamics. The calibration builds on Bayesian optimization, which is a powerful, machine-learning-based tool particularly well suited for computationally expensive numerical optimization. We demonstrate the presented scheme to calibrate the pulse duration as well as the spatial fluence distribution profile of XFEL pulses. Our proposed method can serve as a comprehensive tool for characterizing ultraintense and ultrafast x-ray pulses.

Effect of intense x-ray free-electron laser transient gratings on the magnetic domain structure of Tm:YIG

In ferromagnets, domain patterns can be controlled globally using magnetic fields or spin-polarized currents. In contrast, the local control of the magnetization on the nanometer length scale remains challenging. Here, we demonstrate how magnetic domain patterns in a Tm-doped yttrium iron garnet (Tm:YIG) thin film with perpendicular magnetic anisotropy can be permanently and locally imprinted by high intensity photon pulses of a hard x-ray transient grating (XTG). Micromagnetic simulations provide a qualitative understanding of the observed changes in the orientation of magnetic domains in Tm:YIG and XTG-induced changes. The presented results offer a route for the local manipulation of the magnetic state using hard XTG.

Microfluidic liquid sheets as large-area targets for high repetition XFELs.

The high intensity of X-ray free electron lasers (XFELs) can damage solution-phase samples on every scale, ranging from the molecular or electronic structure of a sample to the macroscopic structure of a liquid microjet. By using a large surface area liquid sheet microjet as a sample target instead of a standard cylindrical microjet, the incident X-ray spot size can be increased such that the incident intensity falls below the damage threshold. This capability is becoming particularly important for high repetition rate XFELs, where destroying a target with each pulse would require prohibitively large volumes of sample. We present here a study of microfluidic liquid sheet dimensions as a function of liquid flow rate. Sheet lengths, widths and thickness gradients are shown for three styles of nozzles fabricated from isotropically etched glass. In-vacuum operation and sample recirculation using these nozzles is demonstrated. The effects of intense XFEL pulses on the structure of a liquid sheet are also briefly examined.

Plasma environmental effects in the atomic structure for simulating x-ray free-electron-laser-heated solid-density matter.

High energy density (HED) matter exists extensively in the Universe, and it can be created with extreme conditions in laboratory facilities such as x-ray free-electron lasers (XFEL). In HED matter, the electronic structure of individual atomic ions is influenced by a dense plasma environment, and one of the most significant phenomena is the ionization potential depression (IPD). Incorporation of the IPD effects is of great importance in accurate modeling of dense plasmas. All theoretical treatments of IPD so far have been based on the assumption of local thermodynamic equilibrium, but its validity is questionable in ultrafast formation dynamics of dense plasmas, particularly when interacting with intense XFEL pulses. A treatment of transient IPD, based on an electronic-structure calculation of an atom in the presence of a plasma environment described by classical particles, has recently been proposed [Phys. Rev. E 103, 023203 (2021)2470-004510.1103/PhysRevE.103.023203], but its application to and impact on plasma dynamics simulations have not been investigated yet. In this work, we extend XMDYN, a hybrid quantum-classical approach combining Monte Carlo and molecular dynamics, by incorporating the proposed IPD treatment into plasma dynamics simulations. We demonstrate the importance of the IPD effects in theoretical modeling of aluminum dense plasmas by comparing two XMDYN simulations: one with electronic-structure calculations of isolated atoms (without IPD) and the other with those of atoms embedded in a plasma (with IPD). At equilibrium, the mean charge obtained in the plasma simulation with IPD is in good agreement with the full quantum-mechanical average-atom model. The present approach promises to be a reliable tool to simulate the creation and nonequilibrium evolution of dense plasmas induced by ultraintense and ultrashort XFEL pulses.

Enhancement of vacuum diffraction by interference of signals produced by a probe x-ray free-electron laser with multiple transverse modes

In this paper, we investigate photon-photon scattering in vacuum in the head-on collision of an optical laser and an x-ray free-electron laser (XFEL) of multiple modes. For the XFEL as probe light with focus waist larger than the optical laser, the scattering photons with the same energy of the initial probe XFEL can be separated from the XFEL background due to the different scattering angle at far field. Here, we study the effect of XFEL's transverse profile, due to superposition of modes, in this vacuum diffraction process. Based on the parameters of upcoming facilities with 100-PW optical lasers and intense XFEL, we show that for a given photon number of the probe XFEL, the separable scattering photon number can be greatly enhanced when the XFEL is composed of different Laguerre-Gaussian modes. As an example, with SHINE's setup there will be 185 photons separable from the XFEL background for each shot, which is 2.5 times that of the case with the usual Gaussian profile.

Calibration methods for charge integrating detectors

Since the introduction of the extremely intense X-ray free electron lasers, the need for low noise, high dynamic range and potentially fast charge integrating detectors has increased significantly. Among all the problems that research and development groups have to face in the development of such detectors, their calibration represents one of the most challenging and the collaboration between the detector development and user groups is of fundamental importance. The main challenge is to develop a calibration suite that is capable to test the detector over a wide dynamic range, with a high granularity and a very high linearity, together with a certain radiation tolerance and the possibility to well define the timings and the synchronization with the detector. Practical considerations have also to be made like the possibility to calibrate the detector in a reasonable time, the availability of the calibration source at the experimental place and so on. Such a calibration test suite is often not represented by a single source but by several sources that can cover different parts of the dynamic range and that need to be cross calibrated to have a final calibration curve. In this respect an essential part of the calibration is also to develop a mathematical model that allows calibrating the entire dynamic range, taking into account features that are calibration source and/or detector specific. The aim of this contribution is to compare the calibration for the AGIPD detector using several calibration sources such as internal current source, backside pulsing, IR pulsed laser, LED light and mono-energetic protons. The mathematical procedure used to calibrate the different sources will be discussed in great detail showing how to take into account a few shortcomings (like pixel coupling) that are common for many charge integrating detectors. This work has been carried out in the frame of the AGIPD project for the European X-ray Free Electron Laser.

Effects of x-ray free-electron laser pulse intensity on the Mn K β 1,3 x-ray emission spectrum in photosystem II-A case study for metalloprotein crystals and solutions.

In the last ten years, x-ray free-electron lasers (XFELs) have been successfully employed to characterize metalloproteins at room temperature using various techniques including x-ray diffraction, scattering, and spectroscopy. The approach has been to outrun the radiation damage by using femtosecond (fs) x-ray pulses. An example of an important and damage sensitive active metal center is the Mn4CaO5 cluster in photosystem II (PS II), the catalytic site of photosynthetic water oxidation. The combination of serial femtosecond x-ray crystallography and Kβ x-ray emission spectroscopy (XES) has proven to be a powerful multimodal approach for simultaneously probing the overall protein structure and the electronic state of the Mn4CaO5 cluster throughout the catalytic (Kok) cycle. As the observed spectral changes in the Mn4CaO5 cluster are very subtle, it is critical to consider the potential effects of the intense XFEL pulses on the Kβ XES signal. We report here a systematic study of the effects of XFEL peak power, beam focus, and dose on the Mn Kβ1,3 XES spectra in PS II over a wide range of pulse parameters collected over seven different experimental runs using both microcrystal and solution PS II samples. Our findings show that for beam intensities ranging from ∼5 × 1015 to 5 × 1017 W/cm2 at a pulse length of ∼35 fs, the spectral effects are small compared to those observed between S-states in the Kok cycle. Our results provide a benchmark for other XFEL-based XES studies on metalloproteins, confirming the viability of this approach.

Ultrafast structural changes in matter induced by intense X-ray free-electron laser pulses

Ultrafast structural changes in matter induced by intense X-ray free-electron laser pulses

Fluorescence intensity correlation imaging with high spatial resolution and elemental contrast using intense x-ray pulses.

We theoretically investigate the fluorescence intensity correlation (FIC) of Ar clusters and Mo-doped iron oxide nanoparticles subjected to intense, femtosecond, and sub-femtosecond x-ray free-electron laser pulses for high-resolution and elemental contrast imaging. We present the FIC of and emission in Ar clusters and discuss the impact of sample damage on retrieving high-resolution structural information and compare the obtained structural information with those from the coherent diffractive imaging (CDI) approach. We found that, while sub-femtosecond pulses will substantially benefit the CDI approach, few-femtosecond pulses may be sufficient for achieving high-resolution information with the FIC. Furthermore, we show that the fluorescence intensity correlation computed from the fluorescence of the Mo atoms in Mo-doped iron oxide nanoparticles can be used to image dopant distributions in the nonresonant regime.

Near-GeV Electron Beams at a Few Per-Mille Level from a Laser Wakefield Accelerator via Density-Tailored Plasma.

A simple, efficient scheme was developed to obtain near-gigaelectronvolt electron beams with energy spreads of few per-mille level in a single-stage laser wakefield accelerator. Longitudinal plasma density was tailored to control relativistic laser-beam evolution, resulting in injection, dechirping, and a quasi-phase-stable acceleration. With this scheme, electron beams with peak energies of 780-840MeV, rms energy spreads of 2.4‰-4.1‰, charges of 8.5-23.6pC, and rms divergences of 0.1-0.4mrad were experimentally obtained. Quasi-three-dimensional particle-in-cell simulations agreed well with the experimental results. The dechirping strength was estimated to reach up to 11 TeV/mm/m, which is higher than previously obtained results. Such high-quality electron beams will boost the development of compact intense coherent radiation sources and x-ray free-electron lasers.

Using X-ray free-electron lasers for spectroscopy of molecular catalysts and metalloenzymes.

The metal centres in metalloenzymes and molecular catalysts are responsible for the rearrangement of atoms and electrons during complex chemical reactions, and they enable selective pathways of charge and spin transfer, bond breaking/making and the formation of new molecules. Mapping the electronic structural changes at the metal sites during the reactions gives a unique mechanistic insight that has been difficult to obtain to date. The development of X-ray free-electron lasers (XFELs) enables powerful new probes of electronic structure dynamics to advance our understanding of metalloenzymes. The ultrashort, intense and tunable XFEL pulses enable X-ray spectroscopic studies of metalloenzymes, molecular catalysts and chemical reactions, under functional conditions and in real time. In this Technical Review, we describe the current state of the art of X-ray spectroscopy studies at XFELs and highlight some new techniques currently under development. With more XFEL facilities starting operation and more in the planning or construction phase, new capabilities are expected, including high repetition rate, better XFEL pulse control and advanced instrumentation. For the first time, it will be possible to make real-time molecular movies of metalloenzymes and catalysts in solution, while chemical reactions are taking place.

Clocking Auger electrons

Intense X-ray free-electron lasers (XFELs) can rapidly excite matter, leaving it in inherently unstable states that decay on femtosecond timescales. As the relaxation occurs primarily via Auger emission, excited state observations are constrained by Auger decay. In situ measurement of this process is therefore crucial, yet it has thus far remained elusive at XFELs due to inherent timing and phase jitter, which can be orders of magnitude larger than the timescale of Auger decay. Here, we develop a new approach termed self-referenced attosecond streaking, based upon simultaneous measurements of streaked photo- and Auger electrons. Our technique enables sub-femtosecond resolution in spite of jitter. We exploit this method to make the first XFEL time-domain measurement of the Auger decay lifetime in atomic neon, and, by using a fully quantum-mechanical description, retrieve a lifetime of $2.2^{ + 0.2}_{ - 0.3}$ fs for the KLL decay channel. Importantly, our technique can be generalised to permit the extension of attosecond time-resolved experiments to all current and future FEL facilities.

Analysis of Multi-Hit Crystals in Serial Synchrotron Crystallography Experiments Using High-Viscosity Injectors

Serial Synchrotron Crystallography (SSX) is rapidly emerging as a promising technique for collecting data for time-resolved structural studies or for performing room temperature micro-crystallography measurements using micro-focused beamlines. SSX is often performed using high frame rate detectors in combination with continuous sample scanning or high-viscosity or liquid jet injectors. When performed using ultra-bright X-ray Free Electron Laser (XFEL) sources serial crystallography typically involves a process known as ’diffract-and-destroy’ where each crystal is measured just once before it is destroyed by the intense XFEL pulse. In SSX, however, particularly when using high-viscosity injectors (HVIs) such as Lipidico, the crystal can be intercepted multiple times by the X-ray beam prior to exiting the interaction region. This has a number of important consequences for SSX including whether these multiple-hits can be incorporated into the data analysis or whether they need to be excluded due to the potential impact of radiation damage. Here, we investigate the occurrence and characteristics of multiple hits on single crystals using SSX with lipidico. SSX data are collected from crystals as they tumble within a high viscous stream of silicone grease flowing through a micro-focused X-ray beam. We confirmed that, using the Eiger 16M, we are able to collect up to 42 frames of data from the same single crystal prior to it leaving the X-ray interaction region. The frequency and occurrence of multiple hits may be controlled by varying the sample flow rate and X-ray beam size. Calculations of the absorbed dose confirm that these crystals are likely to undergo radiation damage but that nonetheless incorporating multiple hits into damage-free data should lead to a significant reduction in the number of crystals required for structural analysis when compared to just looking at a single diffraction pattern from each crystal.

The role of transient resonances for ultra-fast imaging of single sucrose nanoclusters.

Intense x-ray free-electron laser (XFEL) pulses hold great promise for imaging function in nanoscale and biological systems with atomic resolution. So far, however, the spatial resolution obtained from single shot experiments lags averaging static experiments. Here we report on a combined computational and experimental study about ultrafast diffractive imaging of sucrose clusters which are benchmark organic samples. Our theoretical model matches the experimental data from the water window to the keV x-ray regime. The large-scale dynamic scattering calculations reveal that transient phenomena driven by non-linear x-ray interaction are decisive for ultrafast imaging applications. Our study illuminates the complex interplay of the imaging process with the rapidly changing transient electronic structures in XFEL experiments and shows how computational models allow optimization of the parameters for ultrafast imaging experiments.

Electron spectroscopic study of nanoplasma formation triggered by intense soft x-ray pulses.

Using electron spectroscopy, we investigated the nanoplasma formation process generated in xenon clusters by intense soft x-ray free electron laser (FEL) pulses. We found clear FEL intensity dependence of electron spectra. Multistep ionization and subsequent ionization frustration features are evident for the low FEL-intensity region, and the thermal electron emission emerges at the high FEL intensity. The present FEL intensity dependence of the electron spectra is well addressed by the frustration parameter introduced by Arbeiter and Fennel [New J. Phys. 13, 053022 (2011)].

X-ray Spectroscopies of High Energy Density Matter Created with X-ray Free Electron Lasers

The recent progress in the development of X-ray free electron lasers (XFELs) allows for the delivery of over 1011 high-energy photons to solid-density samples in a femtosecond time scale. The corresponding peak brightness of XFEL induces a nonlinear response of matter in a short-wavelength regime. The absorption of an XFEL pulse in a solid also results in the creation of high energy density (HED) matter. The electronic structure and related fundamental properties of such HED matter can be investigated with the control of XFEL and various X-ray spectroscopic techniques. These experimental data provide unique opportunities to benchmark theories and models for extreme conditions and to guide further advances. In this article, the current progress in spectroscopic studies on intense XFEL–matter interactions and HED matter are reviewed, and future research opportunities are discussed.