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A broadband online X‐ray spectrometer has been designed and commissioned at the SUD beamline of the Shanghai Soft X‐ray Free‐Electron Laser Facility, which can deliver both SASE and seeded FEL pulses to user experiments, spanning the photon energy range of 50–620 eV. The resolving powers of the spectrometer calibrated via online measurement at 92 eV and 249 eV are ∼20000 and ∼15000, respectively, and the absolute photon energy is characterized by an electron time‐of‐flight spectrometer. The high energy resolution provided by the spectrometer can differentiate the fine structure in the FEL spectrum, to determine its pulse length. [ABSTRACT FROM AUTHOR]

A broadband online X-ray spectrometer has been designed and commissioned at the SUD beamline of the Shanghai Soft X-ray Free-Electron Laser Facility, which can deliver both SASE and seeded FEL pulses to user experiments, spanning the photon energy range of 50–620 eV. The resolving powers of the spectrometer calibrated via online measurement at 92 eV and 249 eV are ∼20000 and ∼15000, respectively, and the absolute photon energy is characterized by an electron time-of-flight spectrometer. The high energy resolution provided by the spectrometer can differentiate the fine structure in the FEL spectrum, to determine its pulse length.

X-ray gas monitors (XGMs) are operated at the European XFEL for non-invasive single-shot pulse energy measurements and average beam-position monitoring. The underlying measurement principle is the photo-ionization of rare gas atoms at low gas pressures and the detection of the photo-ions and photo-electrons created. These are essential for tuning and sustaining self-amplified spontaneous emission (SASE) operation, machine radiation safety, and sorting single-shot experimental data according to pulse energy. In this paper, the first results from XGM operation at photon energies up to 30 keV are presented, which are far beyond the original specification of this device. Here, the Huge Aperture MultiPlier (HAMP) is used for single-shot pulse energy measurements since the standard X-ray gas monitor detectors (XGMDs) do not provide a sufficient signal-to-noise ratio, even at the highest operating gas pressures. A single-shot correlation coefficient of 0.98 is measured between consecutive XGMs operated with HAMP, which is as good as measuring with the standard XGMD detectors. An intra-train non-linearity of the HAMP signal is discovered, and operation parameters to mitigate this effect are studied. The upper repetition rate limit of HAMP operation at 2.25 MHz is also determined. Finally, the possibilities and limits for future XGM operation at photon energies up to 50 keV are discussed.

This article presents a demonstration of the improved performance of an X-ray free-electron laser (FEL) using the optical klystron mechanism and helical undulator configuration, in comparison with the common planar undulator configuration without optical klystron. The demonstration was carried out at Athos, the soft X-ray beamline of SwissFEL. Athos has variable-polarization undulators, and small magnetic chicanes placed between every two undulators to fully exploit the optical klystron. It was found that, for wavelengths of 1.24 nm and 3.10 nm, the required length to achieve FEL saturation is reduced by about 35% when using both the optical klystron and helical undulators, with each effect accounting for about half of the improvement. Moreover, it is shown that a helical undulator configuration provides a 20% to 50% higher pulse energy than planar undulators. This work represents an important step towards more compact and high-power FELs, rendering this key technology more efficient, affordable and accessible to the scientific community.

This article presents a demonstration of the improved performance of an X‐ray free‐electron laser (FEL) using the optical klystron mechanism and helical undulator configuration, in comparison with the common planar undulator configuration without optical klystron. The demonstration was carried out at Athos, the soft X‐ray beamline of SwissFEL. Athos has variable‐polarization undulators, and small magnetic chicanes placed between every two undulators to fully exploit the optical klystron. It was found that, for wavelengths of 1.24 nm and 3.10 nm, the required length to achieve FEL saturation is reduced by about 35% when using both the optical klystron and helical undulators, with each effect accounting for about half of the improvement. Moreover, it is shown that a helical undulator configuration provides a 20% to 50% higher pulse energy than planar undulators. This work represents an important step towards more compact and high‐power FELs, rendering this key technology more efficient, affordable and accessible to the scientific community. [ABSTRACT FROM AUTHOR]

X‐ray gas monitors (XGMs) are operated at the European XFEL for non‐invasive single‐shot pulse energy measurements and average beam‐position monitoring. The underlying measurement principle is the photo‐ionization of rare gas atoms at low gas pressures and the detection of the photo‐ions and photo‐electrons created. These are essential for tuning and sustaining self‐amplified spontaneous emission (SASE) operation, machine radiation safety, and sorting single‐shot experimental data according to pulse energy. In this paper, the first results from XGM operation at photon energies up to 30 keV are presented, which are far beyond the original specification of this device. Here, the Huge Aperture MultiPlier (HAMP) is used for single‐shot pulse energy measurements since the standard X‐ray gas monitor detectors (XGMDs) do not provide a sufficient signal‐to‐noise ratio, even at the highest operating gas pressures. A single‐shot correlation coefficient of 0.98 is measured between consecutive XGMs operated with HAMP, which is as good as measuring with the standard XGMD detectors. An intra‐train non‐linearity of the HAMP signal is discovered, and operation parameters to mitigate this effect are studied. The upper repetition rate limit of HAMP operation at 2.25 MHz is also determined. Finally, the possibilities and limits for future XGM operation at photon energies up to 50 keV are discussed. [ABSTRACT FROM AUTHOR]

Fixed targets are a popular form of sample-delivery system used in serial crystallography at synchrotron and X-ray free-electron laser sources. They offer a wide range of sample-preparation options and are generally easy to use. The supports are typically made from silicon, quartz or polymer. Of these, currently, only silicon offers the ability to perform an aperture-aligned data collection where crystals are loaded into cavities in precise locations and sequentially rastered through, in step with the X-ray pulses. The polymer-based fixed targets have lacked the precision fabrication to enable this data-collection strategy and have been limited to directed-raster scans with crystals randomly distributed across the polymer surface. Here, the fabrication and first results from a new polymer-based fixed target, the micro-structured polymer fixed targets (MISP chips), are presented. MISP chips, like those made from silicon, have a precise array of cavities and fiducial markers. They consist of a structured polymer membrane and a stabilization frame. Crystals can be loaded into the cavities and the excess crystallization solution removed through apertures at their base. The fiducial markers allow for a rapid calculation of the aperture locations. The chips have a low X-ray background and, since they are optically transparent, also allow for an a priori analysis of crystal locations. This location mapping could, ultimately, optimize hit rates towards 100%. A black version of the MISP chip was produced to reduce light contamination for optical-pump/X-ray probe experiments. A study of the loading properties of the chips reveals that these types of fixed targets are best optimized for crystals of the order of 25 µm, but quality data can be collected from crystals as small as 5 µm. With the development of these chips, it has been proved that polymer-based fixed targets can be made with the precision required for aperture-alignment-based data-collection strategies. Further work can now be directed towards more cost-effective mass fabrication to make their use more sustainable for serial crystallography facilities and users.

In this commentary, we explore the pioneering implementation of 3D-printed thin liquid sheet devices for advanced X-ray scattering and spectroscopy experiments at high-repetition rate XFELs.

X-ray free-electron lasers (XFELs) can probe chemical and biological reactions as they unfold with unprecedented spatial and temporal resolution. A principal challenge in this pursuit involves the delivery of samples to the X-ray interaction point in such a way that produces data of the highest possible quality and with maximal efficiency. This is hampered by intrinsic constraints posed by the light source and operation within a beamline environment. For liquid samples, the solution typically involves some form of high-speed liquid jet, capable of keeping up with the rate of X-ray pulses. However, conventional jets are not ideal because of radiation-induced explosions of the jet, as well as their cylindrical geometry combined with the X-ray pointing instability of many beamlines which causes the interaction volume to differ for every pulse. This complicates data analysis and contributes to measurement errors. An alternative geometry is a liquid sheet jet which, with its constant thickness over large areas, eliminates the problems related to X-ray pointing. Since liquid sheets can be made very thin, the radiation-induced explosion is reduced, boosting their stability. These are especially attractive for experiments which benefit from small interaction volumes such as fluctuation X-ray scattering and several types of spectroscopy. Although their use has increased for soft X-ray applications in recent years, there has not yet been wide-scale adoption at XFELs. Here, gas-accelerated liquid sheet jet sample injection is demonstrated at the European XFEL SPB/SFX nano focus beamline. Its performance relative to a conventional liquid jet is evaluated and superior performance across several key factors has been found. This includes a thickness profile ranging from hundreds of nanometres to 60 nm, a fourfold increase in background stability and favorable radiation-induced explosion dynamics at high repetition rates up to 1.13 MHz. Its minute thickness also suggests that ultrafast single-particle solution scattering is a possibility.

The past, current and planned future developments of X-ray imagers in the Photon-Science Detector Group at DESY-Hamburg is presented. the X-ray imagers are custom developed and tailored to the different X-ray sources in Hamburg, including the storage ring PETRA III/IV; the VUV-soft X-ray free electron laser FLASH, and the European Free-Electron Laser. Each source puts different requirements on the X-ray detectors, which is described in detail, together with the technical solutions implemented. [ABSTRACT FROM AUTHOR]

Transmission measurements of the soft X-ray beamline to the Small Quantum Systems (SQS) scientific instrument at the SASE3 undulator of European XFEL are presented. Measurements are reported for a wide range of photon energies (650 eV to 2400 eV), using X-ray gas monitors as well as a bolometric radiometer. The results are in good agreement with simulations for the beam transport and show a transmission of up to 80% over the whole photon energy range. The contribution of second- and third-harmonic radiation of the soft X-ray undulator is determined at selected photon energies by performing transmission measurements using a gas absorber to provide variable attenuation of the incoming photon flux. A comparison of the results with semi-analytic calculations for the generation of free-electron laser pulses in the SASE3 undulator reveals an influence of apertures along the beam transport on the exact harmonic content to be accounted for at the experiment. The second-harmonic content is measured to be in the range of 0.1% to 0.3%, while the third-harmonic contributed a few percent to the SASE3 emission. For experiments at the SQS instrument, these numbers can be reduced through specific selections of the mirror reflection angles.

One of the challenges facing modern free-electron laser (FEL) facilities is the accurate pulse-to-pulse online measurement of the absolute flux of the X-ray pulses, for use by both machine operators for optimization and users of the photon beam to better understand their data. This manuscript presents a methodology that combines existing slow-measurement methods currently used in gas detectors across the world and fast uncalibrated signals from multipliers, meant for relative flux pulse-to-pulse measurements, which create a shot-to-shot absolute flux measurement through the use of sensor-based conditional triggers and algorithms at SwissFEL.

The past, current and planned future developments of X-ray imagers in the Photon-Science Detector Group at DESY-Hamburg is presented. the X-ray imagers are custom developed and tailored to the different X-ray sources in Hamburg, including the storage ring PETRA III/IV; the VUV-soft X-ray free electron laser FLASH, and the European Free-Electron Laser. Each source puts different requirements on the X-ray detectors, which is described in detail, together with the technical solutions implemented.

ABSTRACTOver the last 20 years, XUV and X-ray free-electron lasers have enabled a wide variety of time-resolved experiments that have dramatically advanced our understanding of ultrafast molecular dynamics on atomic length scales and femtosecond time scales. This review focuses on experimental studies of ultrafast dynamics of atoms and molecules in the gas phase, tracing the development of the field from early proof-of-principle studies to recent pump-probe experiments that elucidate the coupled electronic and nuclear dynamics during photochemical reactions with a temporal resolution that is now extending into the attosecond domain.

The outcomes and timescales of molecular nonadiabatic dynamics are decisively impacted by the quantum coherences generated at localized molecular regions. In time-resolved X-ray diffraction imaging, these coherences create distinct signatures via inelastic photon scattering, but they are buried under much stronger background elastic features. Here, we exploit the rich dynamical information encoded in the inelastic patterns, which we reveal by frequency-dispersed covariance ultrafast powder X-ray diffraction of stochastic X-ray free-electron laser pulses. This is demonstrated for the photoisomerization of azobenzene involving the passage through a conical intersection, where the nuclear wave packet branches and explores different quantum pathways. Snapshots of the coherence dynamics are obtained at high frequency shifts, not accessible with conventional diffraction measurements. These provide access to the timing and to the confined spatial distribution of the valence electrons directly involved in the conical intersection passage. This study can be extended to full three-dimensional imaging of conical intersections with ultrafast X-ray and electron diffraction.

The Small Quantum Systems instrument is one of the six operating instruments of the European XFEL, dedicated to the atomic, molecular and cluster physics communities. The instrument started its user operation at the end of 2018 after a commissioning phase. The design and characterization of the beam transport system are described here. The X-ray optical components of the beamline are detailed, and the beamline performances, transmission and focusing capabilities are reported. It is shown that the X-ray beam can be effectively focused as predicted by ray-tracing simulations. The impact of non-ideal X-ray source conditions on the focusing performances is discussed.

Most crystallographic data processing methods use pixel integration. In serial femtosecond crystallography (SFX), the intricate interaction between the reciprocal lattice point and the Ewald sphere is integrated out by averaging symmetrically equivalent observations recorded across a large number (104-106) of exposures. Although sufficient for generating biological insights, this approach converges slowly, and using it to accurately measure anomalous differences has proved difficult. This report presents a novel approach for increasing the accuracy of structure factors obtained from SFX data. A physical model describing all observed pixels is defined to a degree of complexity such that it can decouple the various contributions to the pixel intensities. Model dependencies include lattice orientation, unit-cell dimensions, mosaic structure, incident photon spectra and structure factor amplitudes. Maximum likelihood estimation is used to optimize all model parameters. The application of prior knowledge that structure factor amplitudes are positive quantities is included in the form of a reparameterization. The method is tested using a synthesized SFX dataset of ytterbium(III) lysozyme, where each X-ray laser pulse energy is centered at 9034 eV. This energy is 100 eV above the Yb3+ L-III absorption edge, so the anomalous difference signal is stable at 10 electrons despite the inherent energy jitter of each femtosecond X-ray laser pulse. This work demonstrates that this approach allows the determination of anomalous structure factors with very high accuracy while requiring an order-of-magnitude fewer shots than conventional integration-based methods would require to achieve similar results.

Transmission measurements of the soft X-ray beamline to the Small Quantum Systems (SQS) scientific instrument at the SASE3 undulator of European XFEL are presented. Measurements are reported for a wide range of photon energies (650 eV to 2400 eV), using X-ray gas monitors as well as a bolometric radiometer. The results are in good agreement with simulations for the beam transport and show a transmission of up to 80% over the whole photon energy range. The contribution of second- and third-harmonic radiation of the soft X-ray undulator is determined at selected photon energies by performing transmission measurements using a gas absorber to provide variable attenuation of the incoming photon flux. A comparison of the results with semi-analytic calculations for the generation of free-electron laser pulses in the SASE3 undulator reveals an influence of apertures along the beam transport on the exact harmonic content to be accounted for at the experiment. The secondharmonic content is measured to be in the range of 0.1% to 0.3%, while the third-harmonic contributed a few percent to the SASE3 emission. For experiments at the SQS instrument, these numbers can be reduced through specific selections of the mirror reflection angles. [ABSTRACT FROM AUTHOR]

Featured Application: Surface plasmon refractometry of conducting surfaces applied in terahertz plasmonic integrated circuits and communication lines. With the intensive development of data transmitting and processing devices in the terahertz (THz) frequency range, an important part of which are integrated plasmonic components and communication lines, it becomes necessary to measure correctly the optical constants of their conductive surfaces. In this paper, we describe a reliable method for determining the effective permittivity εm of a metal surface from the measured characteristics (refractive and absorption indices) of THz surface plasmon polaritons (SPPs). The novelty of the method is the conduction of measurements on a metal surface with a dielectric layer of subwavelength thickness, suppressing the radiative losses of SPPs, which are not taken into account by the SPP dispersion equation. The method is tested on a number of flat "gold sputtering–zinc sulfide layer–air" structures with the use of the THz radiation (λ0 = 141 μm) from the Novosibirsk free electron laser (NovoFEL). The SPP characteristics are determined from interferograms measured with a plasmon Michelson interferometer. It is found that the method allows a significant increase in the accuracy of the εm in comparison with measurements on the same metal surface without a dielectric layer. [ABSTRACT FROM AUTHOR]

One of the challenges facing modern free-electron laser (FEL) facilities is the accurate pulse-to-pulse online measurement of the absolute flux of the X-ray pulses, for use by both machine operators for optimization and users of the photon beam to better understand their data. This manuscript presents a methodology that combines existing slow-measurement methods currently used in gas detectors across the world and fast uncalibrated signals from multipliers, meant for relative flux pulse-to-pulse measurements, which create a shot-to-shot absolute flux measurement through the use of sensor-based conditional triggers and algorithms at SwissFEL. [ABSTRACT FROM AUTHOR]

The Small Quantum Systems instrument is one of the six operating instruments of the European XFEL, dedicated to the atomic, molecular and cluster physics communities. The instrument started its user operation at the end of 2018 after a commissioning phase. The design and characterization of the beam transport system are described here. The X-ray optical components of the beamline are detailed, and the beamline performances, transmission and focusing capabilities are reported. It is shown that the X-ray beam can be effectively focused as predicted by ray-tracing simulations. The impact of non-ideal X-ray source conditions on the focusing performances is discussed. [ABSTRACT FROM AUTHOR]

This introductory article is a synopsis of the status and prospects of particle-beam-driven plasma wakefield acceleration (PWFA). Conceptual and experimental breakthroughs obtained over the last years have initiated a rapid growth of the research field, and increased maturity of underlying technology allows an increasing number of research groups to engage in experimental R&D. We briefly describe the fundamental mechanisms of PWFA, from which its chief attractions arise. Most importantly, this is the capability of extremely rapid acceleration of electrons and positrons at gradients many orders of magnitude larger than in conventional accelerators. This allows the size of accelerator units to be shrunk from the kilometre to metre scale, and possibly the quality of accelerated electron beam output to be improved by orders of magnitude. In turn, such compact and high-quality accelerators are potentially transformative for applications across natural, material and life sciences. This overview provides contextual background for the manuscripts of this issue, resulting from a Theo Murphy meeting held in the summer of 2018. This article is part of the Theo Murphy meeting issue 'Directions in particle beam-driven plasma wakefield acceleration'.

Free superfluid helium droplets constitute a versatile medium for a diverse range of experiments in physics and chemistry that extend from studies of the fundamental laws of superfluid motion to the synthesis of novel nanomaterials. In particular, the emergence of quantum vortices in rotating helium droplets is one of the most dramatic hallmarks of superfluidity and gives detailed access to the wave function describing the quantum liquid. This review provides an introduction to quantum vorticity in helium droplets, followed by a historical account of experiments on vortex visualization in bulk superfluid helium and a more detailed discussion of recent advances in the study of the rotational motion of isolated, nano- to micrometer-scale superfluid helium droplets. Ultrafast X-ray and extreme ultraviolet scattering techniques enabled by X-ray free-electron lasers and high-order harmonic generation in particular have facilitated the in situ detection of droplet shapes and the imaging of vortex structures inside individual, isolated droplets. New applications of helium droplets ranging from studies of quantum phase separations to mechanisms of low-temperature aggregation are discussed.

Serial femtosecond crystallography of two-dimensional membrane-protein crystals at X-ray free-electron lasers has the potential to address the dynamics of functionally relevant large-scale motions, which can be sterically hindered in three-dimensional crystals and suppressed in cryocooled samples. In previous work, diffraction data limited to a two-dimensional reciprocal-space slice were evaluated and it was demonstrated that the low intensity of the diffraction signal can be overcome by collecting highly redundant data, thus enhancing the achievable resolution. Here, the application of a newly developed method to analyze diffraction data covering three reciprocal-space dimensions, extracting the reciprocal-space map of the structure-factor amplitudes, is presented. Despite the low resolution and completeness of the data set, it is shown by molecular replacement that the reconstructed amplitudes carry meaningful structural information. Therefore, it appears that these intrinsic limitations in resolution and completeness from two-dimensional crystal diffraction may be overcome by collecting highly redundant data along the three reciprocal-space axes, thus allowing the measurement of large-scale dynamics in pump-probe experiments.

FLASH is the first soft X-ray FEL user facility, routinely providing brilliant photon beams for users since 2005. The second undulator branch of this facility, FLASH2, is gap-tunable, which allows for testing and using advanced lasing concepts. In particular, we developed a two-color operation mode based on the alternatingly tuned undulator segments (every other segment is tuned to the second wavelength). This scheme is advantageous in comparison with a subsequent generation of two colors in two consecutive sections of the undulator line. First, source positions of the two FEL beams are close to each other which makes it easier to focus them on a sample. Second, the amplification is more efficient in this configuration since the segments with respectively "wrong" wavelength still act as bunchers. We studied operation of this scheme in the regime of small and large separation of tunes (up to a factor of two). We developed new methods for online intensity measurements of the two colors simultaneously that require a combination of two detectors. We also demonstrated our capabilities to measure spectral and temporal properties of two pulses with different wavelengths. [ABSTRACT FROM AUTHOR]

The generation of fully coherent and femtosecond time-scale radiation pulses in the X-ray regime is one of the most common demands of ring-based synchrotron light source users. In this paper, a method that utilizes the recent proposed angular dispersion induced microbunching technique to convert external light from high-harmonic generation (HHG) to coherent light at shorter wavelength is proposed. Numerical simulations using the practical parameters of a diffraction-limited storage ring demonstrate the generation of coherent pulse trains with photon energy as high as 2 keV, pulse duration as short as ∼10 fs and high peak brightness directly from an HHG source at 13 nm.

Previous proof-of-concept measurements on single-layer two-dimensional membrane-protein crystals performed at X-ray free-electron lasers (FELs) have demonstrated that the collection of meaningful diffraction patterns, which is not possible at synchrotrons because of radiation-damage issues, is feasible. Here, the results obtained from the analysis of a thousand single-shot, room-temperature X-ray FEL diffraction images from two-dimensional crystals of a bacteriorhodopsin mutant are reported in detail. The high redundancy in the measurements boosts the intensity signal-to-noise ratio, so that the values of the diffracted intensities can be reliably determined down to the detector-edge resolution of 4 Å. The results show that two-dimensional serial crystallography at X-ray FELs is a suitable method to study membrane proteins to near-atomic length scales at ambient temperature. The method presented here can be extended to pump-probe studies of optically triggered structural changes on submillisecond timescales in two-dimensional crystals, which allow functionally relevant large-scale motions that may be quenched in three-dimensional crystals.

X-ray free-electron lasers (XFELs) have the ability to produce ultra-bright femtosecond X-ray pulses for coherent diffraction imaging of biomolecules. While the development of methods and algorithms for macromolecular crystallography is now mature, XFEL experiments involving aerosolized or solvated biomolecular samples offer new challenges in terms of both experimental design and data processing. Skopi is a simulation package that can generate single-hit diffraction images for reconstruction algorithms, multihit diffraction images of aggregated particles for training machine learning classifiers using labeled data, diffraction images of randomly distributed particles for fluctuation X-ray scattering algorithms, and diffraction images of reference and target particles for holographic reconstruction algorithms. Skopi is a resource to aid feasibility studies and advance the development of algorithms for noncrystalline experiments at XFEL facilities. [ABSTRACT FROM AUTHOR]

The authors present a concurrent Monte Carlo (MC)–molecular dynamics (MD) approach to modeling matter response to excitation of its electronic system at nanometric scales. The two methods are combined on‐the‐fly at each time step in one code, TREKIS‐4. The MC model describes the arrival of irradiation (a photon, an electron, or a fast ion). It traces induced cascades of secondary electrons and holes, and their energy exchange with atoms due to scattering. The excited atomic system is simulated with an MD model. An efficient way is proposed to account for nonthermal effects in the electron‐atom energy transfer in covalent materials via the conversion of the potential energy of the electronic ensemble into the kinetic energy of atoms. Such a combined MC–MD approach enables a time‐resolved tracing of the excitation kinetics of both, the electronic and atomic systems, and their simultaneous response to a deposited dose. As a proof‐of‐principle, it is shown that the proposed method describes atomic dynamics after X‐ray irradiation in good agreement with tight‐binding MD. The model also allows gaining insights into the atomic system behavior during the energy deposition from a nonequilibrium electronic system excited by an ion impact. [ABSTRACT FROM AUTHOR]

Many soft-matter systems are composed of macromolecules or nanoparticles suspended in water. The characteristic times at intrinsic length scales of a few nanometres fall therefore in the microsecond and sub-microsecond time regimes. With the development of free-electron lasers (FELs) and fourth-generation synchrotron light-sources, time-resolved experiments in such time and length ranges will become routinely accessible in the near future. In the present work we report our findings on prototypical soft-matter systems, composed of charge-stabilized silica nanoparticles dispersed in water, with radii between 12 and 15 nm and volume fractions between 0.005 and 0.2. The sample dynamics were probed by means of X-ray photon correlation spectroscopy, employing the megahertz pulse repetition rate of the European XFEL and the Adaptive Gain Integrating Pixel Detector. We show that it is possible to correctly identify the dynamical properties that determine the diffusion constant, both for stationary samples and for systems driven by XFEL pulses. Remarkably, despite the high photon density the only observable induced effect is the heating of the scattering volume, meaning that all other X-ray induced effects do not influence the structure and the dynamics on the probed timescales. This work also illustrates the potential to control such induced heating and it can be predicted with thermodynamic models.

Self-amplified spontaneous-emission (SASE) free-electron lasers (FELs) deliver ultrashort pulses with femtosecond durations. Due to the fluctuating nature of the radiation properties of SASE FELs, characterizing FEL pulses on a single-shot basis is necessary. Therefore, we use terahertz streaking to characterize the temporal properties of ultrashort extreme ultraviolet pulses from the free-electron laser in Hamburg (FLASH). In this study, pulse duration as well as pulse energy are measured in a wavelength range from 8 to 34 nm as functions of undulators contributing to the lasing process. The results are compared to one-dimensional and three-dimensional, time-dependent FEL simulations. [ABSTRACT FROM AUTHOR]

Free-electron lasers (FELs) are the most advanced class of light-sources, by virtue of their unique capability to lase high-brightness pulses characterized by wavelengths spanning the extreme-ultraviolet, the soft and hard X-ray spectral domains, as well as by temporal lengths lying in the femtosecond (fs) timescale. The next step to push the current standards in ultrafast X-ray science is strongly linked to the possibility of engineering and exploiting time-resolved experiments exclusively for FELs pulses, ideally having different colors tunable at specific electronic resonance of the chemical elements. At the seeded FERMI FEL (Trieste, Italy) this goal is committed to the optical device known as AC/DC, which stands for the auto correlator/delay creator. AC/DC is designed to double the incoming FEL pulse splitting the photon beam by inserting a grazing incidence flat mirror, thus preserving the spectral and temporal properties, and further delaying one of these two pulses in time. It can independently tune the FEL pulses fluence on the two optical paths by means of solid-state filters, too. Here, we present a detailed description about this optical device. Strong emphasis is dedicated to the AC/DC opto-mechanical design and to the laser-based feedback systems implemented to compensate for any mismatch affecting the FEL optical trajectory, ascribable to both mechanical imperfections and paraxial errors rising during a temporal delay scan. [ABSTRACT FROM AUTHOR]

There is a great interest in generating high-power hard X-ray Free Electron Laser (FEL) in the terawatt (TW) level that can enable coherent diffraction imaging of complex molecules like proteins and probe fundamental high-field physics. A feasibility study of producing such X-ray pulses was carried out employing a configuration beginning with a Self-Amplified Spontaneous Emission FEL, followed by a “self-seeding” crystal monochromator generating a fully coherent seed, and finishing with a long tapered undulator where the coherent seed recombines with the electron bunch and is amplified to high power. The undulator tapering profile, the phase advance in the undulator break sections, the quadrupole focusing strength, etc. are parameters to be optimized. A Genetic Algorithm (GA) is adopted for this multi-dimensional optimization. Concrete examples are given for LINAC Coherent Light Source (LCLS) and LCLS-II-type systems. Analytical estimate is also developed to cross check the simulation and optimization results as a quick and complimentary tool.

There is a great interest in generating high-power hard X-ray Free Electron Laser (FEL) in the terawatt (TW) level that can enable coherent diffraction imaging of complex molecules like proteins and probe fundamental high-field physics. A feasibility study of producing such X-ray pulses was carried out employing a configuration beginning with a Self-Amplified Spontaneous Emission FEL, followed by a “self-seeding” crystal monochromator generating a fully coherent seed, and finishing with a long tapered undulator where the coherent seed recombines with the electron bunch and is amplified to high power. The undulator tapering profile, the phase advance in the undulator break sections, the quadrupole focusing strength, etc. are parameters to be optimized. A Genetic Algorithm (GA) is adopted for this multi-dimensional optimization. Concrete examples are given for LINAC Coherent Light Source (LCLS) and LCLS-II-type systems. Analytical estimate is also developed to cross check the simulation and optimization results as a quick and complimentary tool.

The generation of fully coherent and femtosecond time‐scale radiation pulses in the X‐ray regime is one of the most common demands of ring‐based synchrotron light source users. In this paper, a method that utilizes the recent proposed angular dispersion induced microbunching technique to convert external light from high‐harmonic generation (HHG) to coherent light at shorter wavelength is proposed. Numerical simulations using the practical parameters of a diffraction‐limited storage ring demonstrate the generation of coherent pulse trains with photon energy as high as 2 keV, pulse duration as short as ∼10 fs and high peak brightness directly from an HHG source at 13 nm. [ABSTRACT FROM AUTHOR]

X-ray free-electron lasers (FELs) deliver ultrabright X-ray pulses, but not the sequences of phase-coherent pulses required for time-domain interferometry and control of quantum states. For conventional split-and-delay schemes to produce such sequences, the challenge stems from extreme stability requirements when splitting Ångstrom wavelength beams, where the tiniest pathlength differences introduce phase jitter. We describe an FEL mode based on selective electron-bunch degradation and transverse beam shaping in the accelerator, combined with a self-seeded photon emission scheme. Instead of splitting the photon pulses after their generation by the FEL,we split the electron bunch in the accelerator, prior to photon generation, to obtain phase-locked X-ray pulses with subfemtosecond duration. Time-domain interferometry becomes possible, enabling the concomitant program of classical and quantum optics experiments with X-rays. The scheme leads to scientific benefits of cutting-edge FELs with attosecond and/or high-repetition rate capabilities, ranging from the X-ray analog of Fourier transform infrared spectroscopy to damage-free measurements. [ABSTRACT FROM AUTHOR]

Free‐electron lasers could enable X‐ray imaging of single biological macromolecules and the study of protein dynamics, paving the way for a powerful new imaging tool in structural biology, but a low signal‐to‐noise ratio and missing regions in the detectors, colloquially termed 'masks', affect data collection and hamper real‐time evaluation of experimental data. In this article, the challenges posed by noise and masks are tackled by introducing a neural network pipeline that aims to restore diffraction intensities. For training and testing of the model, a data set of diffraction patterns was simulated from 10 900 different proteins with molecular weights within the range of 10–100 kDa and collected at a photon energy of 8 keV. The method is compared with a simple low‐pass filtering algorithm based on autocorrelation constraints. The results show an improvement in the mean‐squared error of roughly two orders of magnitude in the presence of masks compared with the noisy data. The algorithm was also tested at increasing mask width, leading to the conclusion that demasking can achieve good results when the mask is smaller than half of the central speckle of the pattern. The results highlight the competitiveness of this model for data processing and the feasibility of restoring diffraction intensities from unknown structures in real time using deep learning methods. Finally, an example is shown of this preprocessing making orientation recovery more reliable, especially for data sets containing very few patterns, using the expansion–maximization–compression algorithm. [ABSTRACT FROM AUTHOR]

Toroidally and spherically bent single crystals are widely employed as optical elements in hard X-ray spectrometry at synchrotron and free-electron laser light sources, and in laboratory-scale instruments. To achieve optimal spectrometer performance, a solid theoretical understanding of the diffraction properties of such crystals is essential. In this work, a general method to calculate the internal stress and strain fields of toroidally bent crystals and how to apply it to predict their diffraction properties is presented. Solutions are derived and discussed for circular and rectangular spherically bent wafers due to their prevalence in contemporary instrumentation.

Most crystallographic data processing methods use pixel integration. In serial femtosecond crystallography (SFX), the intricate interaction between the reciprocal lattice point and the Ewald sphere is integrated out by averaging symmetrically equivalent observations recorded across a large number (104−106) of exposures. Although sufficient for generating biological insights, this approach converges slowly, and using it to accurately measure anomalous differences has proved difficult. This report presents a novel approach for increasing the accuracy of structure factors obtained from SFX data. A physical model describing all observed pixels is defined to a degree of complexity such that it can decouple the various contributions to the pixel intensities. Model dependencies include lattice orientation, unit-cell dimensions, mosaic structure, incident photon spectra and structure factor amplitudes. Maximum likelihood estimation is used to optimize all model parameters. The application of prior knowledge that structure factor amplitudes are positive quantities is included in the form of a reparameterization. The method is tested using a synthesized SFX dataset of ytterbium(III) lysozyme, where each X-ray laser pulse energy is centered at 9034 eV. This energy is 100 eV above the Yb3+ L-III absorption edge, so the anomalous difference signal is stable at 10 electrons despite the inherent energy jitter of each femtosecond X-ray laser pulse. This work demonstrates that this approach allows the determination of anomalous structure factors with very high accuracy while requiring an order-of-magnitude fewer shots than conventional integration-based methods would require to achieve similar results.

Foreword to the virtual issue papers from the PhotonMEADOW2023 workshop., (open access.)