X-ray Free-electron Laser Radiation Research Articles

Spectral Flux Enhancement of X Rays for Addressing Ultranarrow Nuclear Transitions.

Recently, the 1.4 feV ultranarrow nuclear transition at 12.4keV energy in ^{45}Sc was resonantly excited for the first time using radiation from the self-seeded EuXFEL laser [Y. Shvyd'ko et al., Resonant x-ray excitation of the nuclear clock isomer ^{45}Sc, Nature (London) 622, 471 (2023)NATUAS0028-083610.1038/s41586-023-06491-w], establishing ^{45}Sc as a promising candidate for a future Mössbauer nuclear clock. While this experiment demonstrated a high potential of x-ray free-electron laser sources for resonantly exciting nuclear isomers in the hard x-ray range, it also highlighted a severe limitation in the achievable excitation level caused by their extremely large spectral bandwidth ∼1 eV. In this Letter, we propose a method to enhance the spectral flux of x-ray free-electron laser radiation using a resonant absorber with a longitudinal gradient in the nuclear transition frequency. A portion of the incident pulse can be absorbed into a nuclear collective excitation, and converted back into x-ray radiation by reversing the sign of the frequency gradient. Spectral narrowing and flux enhancement of this re-emitted x-ray field is achieved by using a reversed frequency gradient with a smaller magnitude than the initial one. About a hundredfold of such spectral flux enhancement is feasible in ^{45}Sc_{2}O_{3} single crystal, rendering a more efficient source for nuclear excitation and facilitating the experimental observation of resonant fluorescence and coherent forward scattering at the 12.4keV transition, both of which are essential for realizing a nuclear clock.

Ionization by XFEL radiation produces distinct structure in liquid water

In the warm dense matter (WDM) regime, where condensed, gas, and plasma phases coexist, matter frequently exhibits unusual properties that cannot be described by contemporary theory. Experiments reporting phenomena in WDM are therefore of interest to advance our physical understanding of this regime, which is found in dwarf stars, giant planets, and fusion ignition experiments. Using 7.1 keV X-ray free electron laser radiation (nominally 5×105 J/cm2), we produced and probed transient WDM in liquid water. Wide-angle X-ray scattering (WAXS) from the probe reveals a new ~9 Å structure that forms within 75 fs. By 100 fs, the WAXS peak corresponding to this new structure is of comparable magnitude to the ambient water peak, which is attenuated. Simulations suggest that the experiment probes a superposition of two regimes. In the first, fluences expected at the focus severely ionize the water, which becomes effectively transparent to the probe. In the second, out-of-focus pump radiation produces O1+ and O2+ ions, which rearrange due to Coulombic repulsion over 10 s of fs. Our simulations account for a decrease in ambient water signal and an increase in low-angle X-ray scattering but not the experimentally observed 9 Å feature, presenting a new challenge for theory.

Appraising protein conformational changes by resampling time-resolved serial x-ray crystallography data.

With the development of serial crystallography at both x-ray free electron laser and synchrotron radiation sources, time-resolved x-ray crystallography is increasingly being applied to study conformational changes in macromolecules. A successful time-resolved serial crystallography study requires the growth of microcrystals, a mechanism for synchronized and homogeneous excitation of the reaction of interest within microcrystals, and tools for structural interpretation. Here, we utilize time-resolved serial femtosecond crystallography data collected from microcrystals of bacteriorhodopsin to compare results from partial occupancy structural refinement and refinement against extrapolated data. We illustrate the domain wherein the amplitude of refined conformational changes is inversely proportional to the activated state occupancy. We illustrate how resampling strategies allow coordinate uncertainty to be estimated and demonstrate that these two approaches to structural refinement agree within coordinate errors. We illustrate how singular value decomposition of a set of difference Fourier electron density maps calculated from resampled data can minimize phase bias in these maps, and we quantify residual densities for transient water molecules by analyzing difference Fourier and Polder omit maps from resampled data. We suggest that these tools may assist others in judging the confidence with which observed electron density differences may be interpreted as functionally important conformational changes.

Cascaded hard X-ray self-seeded free-electron laser at megahertz repetition rate

AbstractHigh-resolution X-ray spectroscopy in the sub-nanosecond to femtosecond time range requires ultrashort X-ray pulses and a spectral X-ray flux considerably larger than that presently available. X-ray free-electron laser (XFEL) radiation from hard X-ray self-seeding (HXRSS) setups has been demonstrated in the past and offers the necessary peak flux properties. So far, these systems could not provide high repetition rates enabling a high average flux. We report the results for a cascaded HXRSS system installed at the European XFEL, currently the only operating high-repetition-rate hard X-ray XFEL facility worldwide. A high repetition rate, combined with HXRSS, allows the generation of millijoule-level pulses in the photon energy range of 6–14 keV with a bandwidth of around 1 eV (corresponding to about 1 mJ eV–1 peak spectral density) at the rate of ten trains per second, each train including hundreds of pulses arriving at a megahertz repetition rate. At 2.25 MHz repetition rate and photon energies in the 6–7 keV range, we observed and characterized the heat-load effects on the HXRSS crystals, substantially altering the spectra of subsequent X-ray pulses. We demonstrated that our cascaded self-seeding scheme reduces this detrimental effect to below the detection level. This opens up exciting new possibilities in a wide range of scientific fields employing ultrafast X-ray spectroscopy, scattering and imaging techniques.

A phenomenological model of the X-ray pulse statistics of a high-repetition-rate X-ray free-electron laser.

Many coherent imaging applications that utilize ultrafast X-ray free-electron laser (XFEL) radiation pulses are highly sensitive to fluctuations in the shot-to-shot statistical properties of the source. Understanding and modelling these fluctuations are key to successful experiment planning and necessary to maximize the potential of XFEL facilities. Current models of XFEL radiation and their shot-to-shot statistics are based on theoretical descriptions of the source and are limited in their ability to capture the shot-to-shot intensity fluctuations observed experimentally. The lack of accurate temporal statistics in simulations that utilize these models is a significant barrier to optimizing and interpreting data from XFEL coherent diffraction experiments. Presented here is a phenomenological model of XFEL radiation that is capable of capturing the shot-to-shot statistics observed experimentally using a simple time-dependent approximation of the pulse wavefront. The model is applied to reproduce non-stationary shot-to-shot intensity fluctuations observed at the European XFEL, whilst accurately representing the single-shot properties predicted by FEL theory. Compared with previous models, this approach provides a simple, robust and computationally inexpensive method of generating statistical representations of XFEL radiation.

Generation of Large-Bandwidth High-Power X-Ray Free-Electron-Laser Pulses Using a Hollow-Channel Plasma

Large-bandwidth x-ray free-electron-laser (XFEL) facilities are desirable scientific tools in various fields, such as molecular structural dynamics and spectroscopy diagnosis. Various methods are proposed to broaden the FEL spectra. Here, a method is proposed to generate high-power XFEL radiation of tunable spectral bandwidth using plasma wakefield acceleration. An ultrabroad bandwidth is achieved by chirping the electron beam in a hollow-channel plasma without noticeable slice-beam-quality degradation. A dedicated beamline can match the beams with a large energy chirp in the undulators almost without beam loss. Numerical simulations demonstrate that a relative spectral bandwidth (full width) of up to 24% can be obtained with optimized beam and plasma parameters.

Investigating ultrafast structural dynamics using high repetition rate x-ray FEL radiation at European XFEL

European XFEL is an international facility providing hard and soft x-ray free-electron laser radiation for user experiments with a wide range of scientific applications. Its superconducting linear accelerator enables high repetition rate experiments with a broad range of x-ray pulse delivery patterns. The combination of time-resolved experiments, providing access to the time-domain from sub-femtoseconds to milliseconds, with atomic resolution x-ray geometric and electronic structure determination methods is responsible for the bulk of scientific applications of European XFEL. In addition, the extreme x-ray intensities and coherence properties open new methods for studying matter out of equilibrium. After start of operation in 2017, the facility now harvests scientific applications with impact to the challenge areas climate and energy, health, environment and sustainability, and digitalization. Extensions of European XFEL aim to increase performance and capabilities for new scientific applications. An upgrade of the facility in the early 2030s will increase the applicability of European XFEL to solid materials and provide dedicated instruments for improved conditions in specific research fields.

Self-synchronized and cost-effective time-resolved measurements at x-ray free-electron lasers with femtosecond resolution

X-ray free-electron lasers (XFELs), with pulse durations of a few tens of femtoseconds or shorter, are cutting-edge instruments capable of observing structure and dynamics at the atomic scale. Temporal diagnostics are challenging but of fundamental importance for XFEL performance and experiments. In this paper, we demonstrate a method to characterize on a single-shot basis the temporal profile of both the electron beam and the XFEL radiation with femtosecond resolution. The approach consists in streaking the electron beam after the undulator using the wakefields of a corrugated structure. Its merits are arrival time stability and cost-effectiveness. Our method allows access to self-synchronized femtosecond diagnostics to any XFEL facility at low cost.

Methods of Coherent X-Ray Diffraction Imaging

Methods of coherent X-ray diffraction imaging of the spatial structure of noncrystalline objects and nanocrystals (nanostructures) are considered. Particular attention is paid to the methods of scanning-based coherent diffraction imaging (ptychography), visualization based on coherent surface scattering with application of correlation spectroscopy approaches, and specific features of visualization using X-ray free-electron laser radiation. The corresponding data in the literature are analyzed to demonstrate the state of the art of the methods of coherent diffraction imaging and fields of their application.

A compact and cost-effective hard X-ray free-electron laser driven by a high-brightness and low-energy electron beam

We present the first lasing results of SwissFEL, a hard X-ray free-electron laser (FEL) that recently came into operation at the Paul Scherrer Institute in Switzerland. SwissFEL is a very stable, compact and cost-effective X-ray FEL facility driven by a low-energy and ultra-low-emittance electron beam travelling through short-period undulators. It delivers stable hard X-ray FEL radiation at 1-A wavelength with pulse energies of more than 500 μJ, pulse durations of ~30 fs (root mean square) and spectral bandwidth below the per-mil level. Using special configurations, we have produced pulses shorter than 1 fs and, in a different set-up, broadband radiation with an unprecedented bandwidth of ~2%. The extremely small emittance demonstrated at SwissFEL paves the way for even more compact and affordable hard X-ray FELs, potentially boosting the number of facilities worldwide and thereby expanding the population of the scientific community that has access to X-ray FEL radiation. The first lasing results at SwissFEL, an X-ray free-electron laser, are presented, highlighting the facility’s unique capabilities. A general comparison to other major facilities is also provided.

Femtosecond electronic structure response to high intensity XFEL pulses probed by iron X-ray emission spectroscopy

We report the time-resolved femtosecond evolution of the K-shell X-ray emission spectra of iron during high intensity illumination of X-rays in a micron-sized focused hard X-ray free electron laser (XFEL) beam. Detailed pulse length dependent measurements revealed that rapid spectral energy shift and broadening started within the first 10 fs of the X-ray illumination at intensity levels between 1017 and 1018 W cm-2. We attribute these spectral changes to the rapid evolution of high-density photoelectron mediated secondary collisional ionization processes upon the absorption of the incident XFEL radiation. These fast electronic processes, occurring at timescales well within the typical XFEL pulse durations (i.e., tens of fs), set the boundary conditions of the pulse intensity and sample parameters where the widely-accepted ‘probe-before-destroy’ measurement strategy can be adopted for electronic-structure related XFEL experiments.

Multifocus off-axis zone plates for x-ray free-electron laser experiments

X-ray free-electron lasers (XFELs) are paving the way towards new experiments in many scientific fields, such as ultrafast science, nonlinear spectroscopy, and coherent imaging. However, the strong intensity fluctuations inherent to the lasing process in these sources often lead to problems in signal normalization. In order to address this challenge, we designed, fabricated, and characterized diffractive x-ray optics that combine the focusing properties of a Fresnel zone plate with the beam-splitting capability of a grating in a single diffractive optical element. The possibility to split the incident beam into identical copies allows for direct shot-to-shot normalization of the sample signal, thereby greatly enhancing the signal-to-noise ratio in experiments with XFEL radiation. Here we propose two schemes for the design of such diffractive x-ray optical elements for splitting and focusing an incoming beam into up to three foci by merging a grating with a focusing zone plate. By varying the duty cycle of the grating or the relative shift of the Fresnel zone plate structure, we are able to tune the relative intensities of the different diffraction orders to achieve the desired splitting ratios. Experimental confirmation of the design is provided with soft x-ray light (540 eV) and shows a good agreement with calculations, confirming the suitability of this approach for XFEL experiments.

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 a detailed study of the 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.

Thermal loading on self-seeding monochromators in x-ray free electron lasers

One approach to achieve longitudinally coherent hard X-ray free electron laser (XFEL) radiation is to introduce a single-crystal monochromator in the beam path to generate a co-propagating, time-synchronized self-seeding radiation pulse. For modern high-repetition rate XFELs, however, thermal loading on the crystal can degrade the quality of the seed pulse. To assess limitations on the maximum XFEL pulse repetition rate imposed by the seeding crystal, a comprehensive study of thermomechanical, and X-ray diffraction effects within the crystal is presented for two consecutive self-amplified spontaneous emission pulses incident on both reflective and transmissive crystal monochromators.

Soft X-ray diffraction patterns measured by a LiF detector with sub-micrometre resolution and an ultimate dynamic range.

The unique diagnostic possibilities of X-ray diffraction, small X-ray scattering and phase-contrast imaging techniques applied with high-intensity coherent X-ray synchrotron and X-ray free-electron laser radiation can only be fully realized if a sufficient dynamic range and/or spatial resolution of the detector is available. In this work, it is demonstrated that the use of lithium fluoride (LiF) as a photoluminescence (PL) imaging detector allows measuring of an X-ray diffraction image with a dynamic range of ∼107 within the sub-micrometre spatial resolution. At the PETRA III facility, the diffraction pattern created behind a circular aperture with a diameter of 5 µm irradiated by a beam with a photon energy of 500 eV was recorded on a LiF crystal. In the diffraction pattern, the accumulated dose was varied from 1.7 × 105 J cm-3 in the central maximum to 2 × 10-2 J cm-3 in the 16th maximum of diffraction fringes. The period of the last fringe was measured with 0.8 µm width. The PL response of the LiF crystal being used as a detector on the irradiation dose of 500 eV photons was evaluated. For the particular model of laser-scanning confocal microscope Carl Zeiss LSM700, used for the readout of the PL signal, the calibration dependencies on the intensity of photopumping (excitation) radiation (λ = 488 nm) and the gain have been obtained.

Demonstration of Large Bandwidth Hard X-Ray Free-Electron Laser Pulses at SwissFEL.

We have produced hard x-ray free-electron laser (FEL) radiation with unprecedented large bandwidth tunable up to 2%. The experiments have been carried out at SwissFEL, the x-ray FEL facility at the Paul Scherrer Institute in Switzerland. The bandwidth is enhanced by maximizing the energy chirp of the electron beam, which is accomplished by optimizing the compression setup. We demonstrate continuous tunability of the bandwidth with a simple method only requiring a quadrupole magnet. The generation of such broadband FEL pulses will improve the efficiency of many techniques such as x-ray crystallography and spectroscopy, opening the door to significant progress in photon science. It has already been demonstrated that the broadband pulses of SwissFEL are beneficial to enhance the performance of crystallography, and further SwissFEL users plan to exploit this large bandwidth radiation to improve the efficiency of their measurement techniques.

Characterizing the intrinsic properties of individual XFEL pulses via single-particle diffraction.

With each single X-ray pulse having its own characteristics, understanding the individual property of each X-ray free-electron laser (XFEL) pulse is essential for its applications in probing and manipulating specimens as well as in diagnosing the lasing performance. Intensive research using XFEL radiation over the last several years has introduced techniques to characterize the femtosecond XFEL pulses, but a simple characterization scheme, while not requiring ad hoc assumptions, to address multiple aspects of XFEL radiation via a single data collection process is scant. Here, it is shown that single-particle diffraction patterns collected using single XFEL pulses can provide information about the incident photon flux and coherence property simultaneously, and the X-ray beam profile is inferred. The proposed scheme is highly adaptable to most experimental configurations, and will become an essential approach to understanding single X-ray pulses.

Advances in global optimization of high brightness beams

High brightness electron beams play an important role in accelerator-based applications such as driving X-ray free electron laser (FEL) radiation. In this paper, we report on advances in global beam dynamics optimization of an accelerator design using start-to-end simulations and a new parallel multi-objective differential evolution optimization method. The global optimization results in significant improvement of the final electron beam brightness.

Time-resolved studies of metalloproteins using X-ray free electron laser radiation at SACLA

BackgroundThe invention of the X-ray free-electron laser (XFEL) has provided unprecedented new opportunities for structural biology. The advantage of XFEL is an intense pulse of X-rays and a very short pulse duration (<10 fs) promising a damage-free and time-resolved crystallography approach. Scope of reviewRecent time-resolved crystallographic analyses in XFEL facility SACLA are reviewed. Specifically, metalloproteins involved in the essential reactions of bioenergy conversion including photosystem II, cytochrome c oxidase and nitric oxide reductase are described. Major conclusionsXFEL with pump-probe techniques successfully visualized the process of the reaction and the dynamics of a protein. Since the active center of metalloproteins is very sensitive to the X-ray radiation, damage-free structures obtained by XFEL are essential to draw mechanistic conclusions. Methods and tools for sample delivery and reaction initiation are key for successful measurement of the time-resolved data. General significanceXFEL is at the center of approaches to gain insight into complex mechanism of structural dynamics and the reactions catalyzed by biological macromolecules. Further development has been carried out to expand the application of time-resolved X-ray crystallography. This article is part of a Special Issue entitled Novel measurement techniques for visualizing ‘live’ protein molecules.

Fast longitudinal beam dynamics optimization in x-ray free electron laser linear accelerators

A high peak current, flat longitudinal phase space electron beam is desirable for efficient x-ray free electron laser (FEL) radiation in next generation light sources. To attain such a beam requires the extensive design of the linear accelerator (linac) including both linear and nonlinear effects. In this paper, we propose a lumped longitudinal beam dynamics model for fast optimization of the electron beam longitudinal phase space through the accelerator. This model is much faster than available tracking programs and also shows good agreement with the fully three-dimensional element-by-element multi-particle simulations. We applied this model in a parallel multi-objective differential evolution optimization program to an existing LCLS-II superconducting linac design and obtained an optimal solution with significantly higher core peak current than the original design.