Free Electron Laser Research Articles

Design of a kilohertz repetition rate, low-emittance S-band photoinjector

Low-emittance photoinjector-enabled cutting-edge scientific instruments, such as free-electron lasers, inverse Compton scattering light sources, and ultrafast electron diffraction, will greatly benefit from the improved repetition rate. In this paper, we proposed a specifically designed S-band radio frequency (RF) photoinjector to obtain low emittance and kilohertz (kHz) high-repetition rates simultaneously. By lowering the gradient, much lower RF power is needed to feed the electron gun, and then the heat problem is much easier to handle. Meanwhile, by optimizing the length of the gun’s first cell from the normal case of 0.6-cell to 0.4-cell, the launch phase and the extraction field are significantly improved, thus ensuring the generation of low-emittance electron beams. In our design, the proposed 1.4-cell RF gun can work effectively under different field gradients ranging from 30 MV/m to 100 MV/m. For a standard case of 60 MV/m, 2.5 MW peak RF power with μs level pulse width is sufficient, thus offering the feasibility of improving the repetition rate to kHz level with a standard 5 MW irradiation klystron. In addition, simulated electron beams with a low emittance of 0.29 mm.mrad@200 pC can be generated by this proposed photoinjector, showing that this high-repetition rate injector holds the potential to deliver high-quality beams comparable to those of state-of-the-art S-band photoinjectors. Combining the merits of low emittance and high-repetition rate, this proposed photoinjector will provide a new possibility for future free-electron laser facilities operating at repetition rates ranging from kHz to tens of kHz.

X-ray beam diagnostics at the MID instrument of the European X-ray Free-Electron Laser Facility.

The Materials Imaging and Dynamics (MID) instrument at the European X-ray Free-Electron Laser Facility (EuXFEL) is equipped with a multipurpose diagnostic end-station (DES) at the end of the instrument. The imager unit in DES is a key tool for aligning the beam to a standard trajectory and for adjusting optical elements such as focusing lenses or the split-and-delay line. Furthermore, the DES features a bent-diamond-crystal spectrometer to disperse the spectrum of the direct beam to a line detector. This enables pulse-resolved characterization of the EuXFEL spectrum to provide X-ray energy calibration, and the spectrometer is particularly useful in commissioning special modes of the accelerator. Together with diamond-based intensity monitors, the imager and spectrometer form the DES unit which also contains a heavy-duty beamstop at the end of the MID instrument. Here, we describe the setup in detail and provide exemplary beam diagnostic results.

Coherent diffractive imaging with twisted X-rays: Principles, applications, and outlook

Recent technological breakthroughs in synchrotron and x-ray free electron laser facilities have revolutionized nanoscale structural and dynamic analyses in condensed matter systems. This review provides a comprehensive overview of the advancements in coherent scattering and diffractive imaging techniques, which are now at the forefront of exploring materials science complexities. These techniques, notably Bragg coherent diffractive imaging and x-ray photon correlation spectroscopy, x-ray magnetic dichroism, and x-ray correlation analysis leverage beam coherence to achieve volumetric three-dimensional imaging at unprecedented sub-nanometer resolutions and explore dynamic phenomena within sub-millisecond timeframes. Such capabilities are critical in understanding and developing advanced materials and technologies. Simultaneously, the emergence of chiral crystals—characterized by their unique absence of standard inversion, mirror, or other roto-inversion symmetries—presents both challenges and opportunities. These materials exhibit distinctive interactions with light, leading to phenomena such as molecular optical activity, chiral photonic waveguides, and valley-specific light emissions, which are pivotal in the burgeoning fields of photonic and spintronic devices. This review elucidates how novel x-ray probes can be leveraged to unravel these properties and their implications for future technological applications. A significant focus of this review is the exploration of new avenues in research, particularly the shift from conventional methods to more innovative approaches in studying these chiral materials. Inspired by structured optical beams, the potential of coherent scattering techniques utilizing twisted x-ray beams is examined. This promising direction not only offers higher spatial resolution but also opens the door to previously unattainable insights in materials science. By contextualizing these advancements within the broader scientific landscape and highlighting their practical applications, this review aims to chart a course for future research in this rapidly evolving field.

An experimental application of machine learning algorithms to optimize the FEL lasing via beam trajectory tuning at Dalian Coherent Light Source

The lasing optimization of Free-Electron Laser (FEL) facilities is a time-consuming and challenging task. Instead of operating manually by experienced operators, implementation of machine learning algorithms offers a rapid and adaptable approach for FEL lasing optimization. Recently, such an experiment has been conducted at the vacuum ultraviolet FEL facility - Dalian Coherent Light Source (DCLS). Four algorithms, namely the standard and the neural network-based genetic algorithms, the deep deterministic policy gradient and the soft actor critic reinforcement learning algorithms, have been employed to enhance the FEL intensity by optimizing the electron beam trajectory. These algorithms have shown notable efficacy in enhancing the FEL lasing, especially the reinforcement learning ones which achieved convergence within only approximately 400 iterations. This study demonstrates the validity of machine learning algorithms for FEL lasing optimization, providing a forward-looking perspective on the automatic operation of DCLS.

A 5.12-Gbps serializer circuit for front-end fast readout electronics of silicon pixelated detectors

Advanced synchrotron radiation sources are major facilities for analyzing the formation and evolution of material structure in multidisciplinary research, owing to their high luminosity, low emittance, wide energy bandwidth and other characteristics. In China, several advanced synchrotron radiation sources are under construction, including the HEPS (High Energy Photon Source) and SHINE (Shanghai high repetition rate X-ray Free Electron Laser and extreme light facility). These facilities are poised to become major multidisciplinary research platforms in China. To meet the requirements of pixel detectors in these facilities, dedicated pixel readout chips are being developed, including HEPS-BPIX and HYLITE. This paper presents a high-speed serializer circuit developed in a commercial 130-nm CMOS technology for the full-scale (128 × 128) pixel readout chip of HYLITE, which requires a data rate of 4 Gbps currently. The serializer consists of a 16-to-1 binary-tree multiplexer, a ring-oscillating-based phase-locked loop (RO-PLL) and a current-mode logic driving stage with a multi-stage pre-amplifier. Test results demonstrate its expected functionality within a wide operating range from 0.52 Gbps to 5.5 Gbps. At 5.12 Gbps, the measured jitter values are about 2 ps for random jitter, 20 ps for deterministic jitter, and 47 ps for total jitter with a 10−12 bit error rate. Additionally, the horizontal and vertical eye openings are 0.84 UI and 72%, respectively. These positive results indicate that the serializer meets the requirements of HYLITE.

Slice emittance measurements using a slit-grid system and a fast wall-current monitor.

The time evolution of beam properties in an electron bunch with the duration of a nanosecond was measured with a time resolution of several tens of picoseconds. A combination of horizontal and vertical slits cuts the beamlet from the original beam, with the current waveform of the beamlet measured using a fast wall-current monitor. The reconstruction of the waveform data obtained by scanning these two slits over the entire beam area provided the time evolution of the spatial profile. A similar measurement using two horizontal (vertical) slits separated by a certain distance also provides the time evolution of the phase-space profile. Using this method, the initial beam extracted from the CeB6 thermionic electron gun of the x-ray free-electron laser (XFEL) SACLA was evaluated. Although the slice emittance in the bunch was measured to be constant, the centroid of the spatial profile moved in the transverse direction by a few hundred micrometers in the 0.6ns flat-top region. This movement arises from the temporal variation in the rectangular high-voltage pulse of the beam chopper and can cause an increase in the projected emittance. These measurements are important for evaluating the conditions of the initial beam emitted from the cathode and processed downstream of the gun. Hence, the proposed diagnostic system will play an important role in developing an extremely low-emittance electron beam or an artificial electron beam with a multi-bunch or micro-bunch structure that enhances the brightness of the XFEL light.

Optimized design and characterization of HYLITE, a charge-integration readout chip of XFEL

HYLITE (High dYnamic range free electron Laser Imaging deTEctor) is a charge-integration pixel readout chip designed for SHINE (Shanghai HIgh repetition rate XFEL aNd Extreme light facility). The target specifications for the full-size HYLITE chip include a pixel matrix of 128 × 128 pixels and a frame rate of 10 kHz. In order to meet these specifications, two small-scale chips, designated HYLITE0.1 and HYLITE0.2, were fabricated and underwent comprehensive testing. Some issues were discovered during tests including the noise performance and the error of output ADU (Analog Digital Units) codes.The HYLITE200S represents the third prototype chip developed to address the above issues. The CDS (Correlated Double Sampling) circuits and glitch-clear clock structures are integrated in pixels. Furthermore, to meet the data output rate requirements of the full-size chip, a high-speed data interface has been designed. Test results show that the signal-to-noise ratio is improved to 9.31 for a 12 keV single photon, and the ADU error is fixed. By integrating a phase-locked loop and a balanced encoding logic, the data interface can work steadily at a speed of 3.125 Gbps.

Attosecond analysis illuminates a watery mystery

With powerful x-ray free-electron lasers, researchers are making great strides in ultrafast spectroscopy—with lessons about how molecules arrange themselves at rest.

Changes in an enzyme ensemble during catalysis observed by high-resolution XFEL crystallography.

Enzymes populate ensembles of structures necessary for catalysis that are difficult to experimentally characterize. We use time-resolved mix-and-inject serial crystallography at an x-ray free electron laser to observe catalysis in a designed mutant isocyanide hydratase (ICH) enzyme that enhances sampling of important minor conformations. The active site exists in a mixture of conformations, and formation of the thioimidate intermediate selects for catalytically competent substates. The influence of cysteine ionization on the ICH ensemble is validated by determining structures of the enzyme at multiple pH values. Large molecular dynamics simulations in crystallo and time-resolved electron density maps show that Asp17 ionizes during catalysis and causes conformational changes that propagate across the dimer, permitting water to enter the active site for intermediate hydrolysis. ICH exhibits a tight coupling between ionization of active site residues and catalysis-activated protein motions, exemplifying a mechanism of electrostatic control of enzyme dynamics.

Efficient prediction of attosecond two-colour pulses from an X-ray free-electron laser with machine learning

X-ray free-electron lasers are sources of coherent, high-intensity X-rays with numerous applications in ultra-fast measurements and dynamic structural imaging. Due to the stochastic nature of the self-amplified spontaneous emission process and the difficulty in controlling injection of electrons, output pulses exhibit significant noise and limited temporal coherence. Standard measurement techniques used for characterizing two-coloured X-ray pulses are challenging, as they are either invasive or diagnostically expensive. In this work, we employ machine learning methods such as neural networks and decision trees to predict the central photon energies of pairs of attosecond fundamental and second harmonic pulses using parameters that are easily recorded at the high-repetition rate of a single shot. Using real experimental data, we apply a detailed feature analysis on the input parameters while optimizing the training time of the machine learning methods. Our predictive models are able to make predictions of central photon energy for one of the pulses without measuring the other pulse, thereby leveraging the use of the spectrometer without having to extend its detection window. We anticipate applications in X-ray spectroscopy using XFELs, such as in time-resolved X-ray absorption and photoemission spectroscopy, where improved measurement of input spectra will lead to better experimental outcomes.

Robust image descriptor for machine learning based data reduction in serial crystallography.

Serial crystallography experiments at synchrotron and X-ray free-electron laser (XFEL) sources are producing crystallographic data sets of ever-increasing volume. While these experiments have large data sets and high-frame-rate detectors (around 3520 frames per second), only a small percentage of the data are useful for downstream analysis. Thus, an efficient and real-time data classification pipeline is essential to differentiate reliably between useful and non-useful images, typically known as 'hit' and 'miss', respectively, and keep only hit images on disk for further analysis such as peak finding and indexing. While feature-point extraction is a key component of modern approaches to image classification, existing approaches require computationally expensive patch preprocessing to handle perspective distortion. This paper proposes a pipeline to categorize the data, consisting of a real-time feature extraction algorithm called modified and parallelized FAST (MP-FAST), an image descriptor and a machine learning classifier. For parallelizing the primary operations of the proposed pipeline, central processing units, graphics processing units and field-programmable gate arrays are implemented and their performances compared. Finally, MP-FAST-based image classification is evaluated using a multi-layer perceptron on various data sets, including both synthetic and experimental data. This approach demonstrates superior performance compared with other feature extractors and classifiers.

The CompactLight Design Study

AbstractCompactLight is a Design Study funded by the European Union under the Horizon 2020 research and innovation funding programme, with Grant Agreement No. 777431. CompactLight was conducted by an International Collaboration of 23 international laboratories and academic institutions, three private companies, and five third parties. The project, which started in January 2018 with a duration of 48 months, aimed to design an innovative, compact, and cost-effective hard X-ray FEL facility complemented by a soft X-ray source to pave the road for future compact accelerator-based facilities. The result is an accelerator that can be operated at up to 1 kHz pulse repetition rate, beyond today’s state of the art, using the latest concepts for high brightness electron photoinjectors, very high gradient accelerating structures in X-band, and novel short-period undulators. In this report, we summarize the main deliverable of the project: the CompactLight Conceptual Design Report, which overviews the current status of the design and addresses the main technological challenges.

Improving the Quality of Spontaneously Growing HviGH11 Crystals by Increasing the Viscosity Using Polyethylene Glycols

Proteins can form crystals spontaneously without crystallization experiments. These crystals can be used to determine three-dimensional structures. However, when X-ray diffraction is poor, crystal optimization is required to obtain a high-resolution crystal structure. Endo-1,4-β-xylanase from the fungus Hypocrea virens (HviGH11) spontaneously formed microcrystals after affinity purification and concentration; however, most HviGH11 microcrystals showed poor diffraction in the synchrotron X-ray and X-ray free-electron laser, so a complete three-dimensional structure could not be obtained. This study presents a method to improve the crystal quality of spontaneously grown HviGH11 microcrystals. The crystallization screening results revealed that temperature, pH, and salt were not crucial factors in increasing the solubility or preventing the spontaneous crystal growth of HviGH11. Conversely, the addition of polyethylene glycols (PEGs) as a precipitant facilitated the growth of larger HviGH11 crystals. The improved large HviGH11 crystal showed a diffraction of up to 1.95 Å when exposed to synchrotron X-rays, providing a complete three-dimensional structural dataset. Based on the nucleation rate equation, it was suggested that PEG increases the viscosity of the protein solution rather than promoting nucleation. This increase in viscosity reduced nucleation and facilitated the growth of larger HviGH11 crystals. These results provide valuable insights for future experiments aimed at increasing the size of spontaneously grown crystals.

Simulations of dislocation contrast in dark-field X-ray microscopy.

Dark-field X-ray microscopy (DFXM) is a full-field imaging technique that non-destructively maps the structure and local strain inside deeply embedded crystalline elements in three dimensions. In DFXM, an objective lens is placed along the diffracted beam to generate a magnified projection image of the local diffracted volume. This work explores contrast methods and optimizes the DFXM setup specifically for the case of mapping dislocations. Forward projections of detector images are generated using two complementary simulation tools based on geometrical optics and wavefront propagation, respectively. Weak and strong beam contrast and the mapping of strain components are studied. The feasibility of observing dislocations in a wall is elucidated as a function of the distance between neighbouring dislocations and the spatial resolution. Dislocation studies should be feasible with energy band widths of 10-2, of relevance for fourth-generation synchrotron and X-ray free-electron laser sources.

Generation of interferometrically stable pulse pairs from a free-electron laser using a birefringent interferometer

We present a compact, intrinsically stable common path interferometer for the seeding of free-electron lasers (FELs). The interferometer can handle the required ultraviolet seed wavelengths and features an excellent phase stability of 10 mrad at 265 nm. By seeding the FEL FERMI, we demonstrate the generation of extreme ultraviolet (XUV) pulse pairs with tunable delay and a delay stability of 6 as at 52.5 nm. Prospective applications are Fourier transform spectroscopy, nonlinear spectroscopy and coherent control experiments in the XUV and x-ray domain.

Enhanced EMC-Advantages of partially known orientations in x-ray single particle imaging.

Single particle imaging of proteins in the gas phase with x-ray free-electron lasers holds great potential to study fast protein dynamics, but is currently limited by weak and noisy data. A further challenge is to discover the proteins' orientation as each protein is randomly oriented when exposed to x-rays. Algorithms such as the expand, maximize, and compress (EMC) exist that can solve the orientation problem and reconstruct the three-dimensional diffraction intensity space, given sufficient measurements. If information about orientation were known, for example, by using an electric field to orient the particles, the reconstruction would benefit and potentially reach better results. We used simulated diffraction experiments to test how the reconstructions from EMC improve with particles' orientation to a preferred axis. Our reconstructions converged to correct maps of the three-dimensional diffraction space with fewer measurements if biased orientation information was considered. Even for a moderate bias, there was still significant improvement. Biased orientations also substantially improved the results in the case of missing central information, in particular in the case of small datasets. The effects were even more significant when adding a background with 50% the strength of the averaged diffraction signal photons to the diffraction patterns, sometimes reducing the data requirement for convergence by a factor of 10. This demonstrates the usefulness of having biased orientation information in single particle imaging experiments, even for a weaker bias than what was previously known. This could be a key component in overcoming the problems with background noise that currently plague these experiments.

Differentiating Three-Dimensional Molecular Structures Using Laser-Induced Coulomb Explosion Imaging.

Coulomb explosion imaging (CEI) with x-ray free electron lasers has recently been shown to be a powerful method for obtaining detailed structural information of gas-phase planar ring molecules [R. Boll et al., X-ray multiphoton-induced Coulomb explosion images complex single molecules, Nat. Phys. 18, 423 (2022).NPAHAX1745-247310.1038/s41567-022-01507-0]. In this Letter, we investigate the potential of CEI driven by a tabletop laser and extend this approach to differentiating three-dimensional structures. We study the static CEI patterns of planar and nonplanar organic molecules that resemble the structures of typical products formed in ring-opening reactions. Our results reveal that each molecule exhibits a well-localized and distinctive pattern in three-dimensional fragment-ion momentum space. We find that these patterns yield direct information about the molecular structures and can be qualitatively reproduced using a classical Coulomb explosion simulation. Our findings suggest that laser-induced CEI can serve as a robust method for differentiating molecular structures of organic ring and chain molecules. As such, it holds great promise as a method for following ultrafast structural changes, e.g., during ring-opening reactions, by tracking the motion of individual atoms in pump-probe experiments.

Structural dynamics and functional cooperativity of human NQO1 by ambient temperature serial crystallography and simulations.

The human NQO1 (hNQO1) is a flavin adenine nucleotide (FAD)-dependent oxidoreductase that catalyzes the two-electron reduction of quinones to hydroquinones, being essential for the antioxidant defense system, stabilization of tumor suppressors, and activation of quinone-based chemotherapeutics. Moreover, it is overexpressed in several tumors, which makes it an attractive cancer drug target. To decipher new structural insights into the flavin reductive half-reaction of the catalytic mechanism of hNQO1, we have carried serial crystallography experiments at new ID29 beamline of the ESRF to determine, to the best of our knowledge, the first structure of the hNQO1 in complex with NADH. We have also performed molecular dynamics simulations of free hNQO1 and in complex with NADH. This is the first structural evidence that the hNQO1 functional cooperativity is driven by structural communication between the active sites through long-range propagation of cooperative effects across the hNQO1 structure. Both structural results and MD simulations have supported that the binding of NADH significantly decreases protein dynamics and stabilizes hNQO1 especially at the dimer core and interface. Altogether, these results pave the way for future time-resolved studies, both at x-ray free-electron lasers and synchrotrons, of the dynamics of hNQO1 upon binding to NADH as well as during the FAD cofactor reductive half-reaction. This knowledge will allow us to reveal unprecedented structural information of the relevance of the dynamics during the catalytic function of hNQO1.

Accelerating the convergence of free electron laser simulations by retrieving a spatially coherent component of microbunching

Accelerating the convergence of free electron laser simulations by retrieving a spatially coherent component of microbunching

High-resolution ptychographic imaging at a seeded free-electron laser source using OAM beams

Electromagnetic waves possessing orbital angular momentum (OAM) are powerful tools for applications in optical communications, quantum technologies, and optical tweezers. Recently, they have attracted growing interest since they can be harnessed to detect peculiar helical dichroic effects in chiral molecular media and in magnetic nanostructures. In this work, we perform single-shot per position ptychography on a nanostructured object at a seeded free-electron laser, using extreme ultraviolet OAM beams of different topological charge orders ℓ generated with spiral zone plates. By controlling ℓ, we demonstrate how the structural features of OAM beam profiles determine an improvement of about 30% in image resolution with respect to conventional Gaussian beam illumination. This result extends the capabilities of coherent diffraction imaging techniques, and paves the way for achieving time-resolved high-resolution (below 100 nm) microscopy on large area samples.