Hard X-ray Free Electron Laser Research Articles

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

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

Evidence for phonon hardening in laser-excited gold using x-ray diffraction at a hard x-ray free electron laser

Studies of laser-heated materials on femtosecond timescales have shown that the interatomic potential can be perturbed at sufficiently high laser intensities. For gold, it has been postulated to undergo a strong stiffening leading to an increase of the phonon energies, known as phonon hardening. Despite efforts to investigate this behavior, only measurements at low absorbed energy density have been performed, for which the interpretation of the experimental data remains ambiguous. By using in situ single-shot x-ray diffraction at a hard x-ray free-electron laser, the evolution of diffraction line intensities of laser-excited Au to a higher energy density provides evidence for phonon hardening.

Operation of 2 K cryogenic system with cold compressors for the SHINE test facility

The Shanghai high repetition rate X-ray free electron laser (XFEL) and extreme light facility (SHINE), a quasi-continuous wave hard XFEL facility, is currently under construction. In order to test all the superconducting components, assembled cryomodules and undulators, the SHINE test facility that consists of various test benches has been built. A superfluid cryoplant with 1 kW@2K was installed, commissioned, acceptance tested and turned into operation to support the cryogenic tests. The plant consists not only of a standard compressor system and cold box but also of a process vacuum system for 2 K operation. In the 2 K cryogenic system, three-stage cold compressors are firstly used to compress helium vapor at a mass flow of up to 50 g/s from 28 mbar to about 400 mbar. Afterwards, the sub-atmospheric helium is continually pressurize to the suction pressure of the warm compressors by five parallel process vacuum pumps. During the first eight months of 2 K operations, the tuning of the cold compressor regulation has been implemented to adapt the different static and dynamic heat loads. A helium pressure stability of superconducting cavities better than ±0.15 mbar at 31 mbar was achieved inside the vertical test bench with additional heating power of 160 W. In this paper, the pump down procedure and the operation results of cryogenic system at 2 K will be described.

Correlation of refractive index based and THz streaking arrival time tools for a hard X-ray free-electron laser.

To fully exploit ultra-short X-ray pulse durations routinely available at X-ray free-electron lasers to follow out-of-equilibrium dynamics, inherent arrival time fluctuations of the X-ray pulse with an external perturbing laser pulse need to be measured. In this work, two methods of arrival time measurement were compared to measure the arrival time jitter of hard X-ray pulses. The methods were photoelectron streaking by a THz field and a transient refractive index change of a semiconductor. The methods were validated by shot-to-shot correction of a pump-probe transient reflectivity measurement. An ultimate shot-to-shot full width at half-maximum error between the devices of 19.2 ± 0.1 fs was measured.

A versatile pressure-cell design for studying ultrafast molecular-dynamics in supercritical fluids using coherent multi-pulse x-ray scattering.

Supercritical fluids (SCFs) can be found in a variety of environmental and industrial processes. They exhibit an anomalous thermodynamic behavior, which originates from their fluctuating heterogeneous micro-structure. Characterizing the dynamics of these fluids at high temperature and high pressure with nanometer spatial and picosecond temporal resolution has been very challenging. The advent of hard x-ray free electron lasers has enabled the development of novel multi-pulse ultrafast x-ray scattering techniques, such as x-ray photon correlation spectroscopy (XPCS) and x-ray pump x-ray probe (XPXP). These techniques offer new opportunities for resolving the ultrafast microscopic behavior in SCFs at unprecedented spatiotemporal resolution, unraveling the dynamics of their micro-structure. However, harnessing these capabilities requires a bespoke high-pressure and high-temperature sample system that is optimized to maximize signal intensity and address instrument-specific challenges, such as drift in beamline components, x-ray scattering background, and multi-x-ray-beam overlap. We present a pressure cell compatible with a wide range of SCFs with built-in optical access for XPCS and XPXP and discuss critical aspects of the pressure cell design, with a particular focus on the design optimization for XPCS.

Toward a fully coherent tender and hard X-ray free-electron laser via cascaded EEHG in fourth-generation synchrotron light sources.

Free-electron-laser-based beamlines utilize fully coherent laser pulses with extremely narrow bandwidth allowing direct use of X-rays without monochromators. This could be very beneficial for all users of current and future fourth-generation diffraction-limited synchrotron light sources (DL-SLSs) who need narrowband full-coherence high-brightness X-ray pulses. Based on our previous finding, i.e. that separating the two stages of echo-enabled harmonic generation (EEHG) with a few extra bending-magnet sections provides an effective way to increase the momentum compaction of chicane 1, one can simultaneously achieve adequate prebunching at extremely high harmonics as well as keep the energy modulation to the ideal minimum. This could open the door for cascaded EEHG, toward fully coherent tender and hard X-ray wavelengths. Built on our compact design of a twin-pulse seeding electron beam with an adjustable delay and timing jitter at the level of a few femtoseconds, a cascaded EEHG can be implemented, which includes two EEHG beamlines, where the radiation pulse generated by the first beamline with harmonic h1 could be used as the input seed laser pulse to the second beamline with harmonic h2. Hence, the second radiator could potentially reach very high harmonics [h = h1(20)h2(25-100)] from 500 to 2000, corresponding to tender and hard X-ray wavelengths. It is demonstrated that the cascaded EEHG scheme is compatible with almost any current or planned fourth-generation DL-SLS, with significant benefits for space-limited storage rings in particular. The main advantage is that this scheme requires almost no change of the storage-ring lattice and is fully compatible with other beamlines. Current proposals for rings with much longer straight sections would add self-amplified spontaneous emission as another viable option for storage-ring-based free-electron lasers.

Imaging via Correlation of X-Ray Fluorescence Photons.

We demonstrate that x-ray fluorescence emission, which cannot maintain a stationary interference pattern, can be used to obtain images of structures by recording photon-photon correlations in the manner of the stellar intensity interferometry of Hanbury Brown and Twiss. This is achieved utilizing femtosecond-duration pulses of a hard x-ray free-electron laser to generate the emission in exposures comparable to the coherence time of the fluorescence. Iterative phasing of the photon correlation map generated a model-free real-space image of the structure of the emitters. Since fluorescence can dominate coherent scattering, this may enable imaging uncrystallised macromolecules.

Frequency and spatially chirped free-electron laser pulses

We have produced hard x-ray free-electron laser (FEL) pulses, which are chirped both in photon energy and in spatial position. The experiments have been carried out at the hard x-ray beamline Aramis at SwissFEL, located at the Paul Scherrer Institute in Switzerland. The FEL beamline was operated without any external focusing and with a tilted, energy-chirped electron bunch, whose properties are then transferred to the photon beam. The resulting FEL pulses were used for a single-shot absorption x-ray spectroscopy experiment at the Alvra endstation. But, as will be outlined, applications of this type of tailored FEL pulse go beyond such experiments, allowing for x-ray pulse compression and control of the transverse coherence within the pulse.Received 13 May 2022Accepted 22 February 2023DOI:https://doi.org/10.1103/PhysRevResearch.5.L022009Published by the American Physical Society under the terms of the Creative Commons Attribution 4.0 International license. Further distribution of this work must maintain attribution to the author(s) and the published article's title, journal citation, and DOI.Published by the American Physical SocietyPhysics Subject Headings (PhySH)Physical SystemsFree-electron lasersAccelerators & Beams

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.

Arrival time diagnosis method of high refrequency hard X-ray free electron laser

X-ray free electron laser (XFEL) pulse time diagnosis technology is often used to detect the relative arrival time of XFEL pulse and auxiliary laser near the experimental station. It is an important auxiliary technology and provides a reference signal for the pump-probe pulse in the XFEL laser pump-probe experiment. With the development of XFEL towards high repetition frequency and short pulse, higher requirements are put forward for diagnostic frequency, pump sample and resolution in time diagnosis. The technology is realized by the pump-probe method and optical cross-correlation method. When the XFEL pulse is incident on the high-bandwidth semiconductor solid target instantaneously, the complex refractive index of the solid target will change, then the arrival time of XFEL will be encoded in the mutation space. In thiswork, we design an XFEL pulse arrival time diagnostic device based on two methods: spatial coding and spectral coding. In this framework, the interaction between X-ray and solid target is explored by Beer's absorption theory and atomic scattering theory. Therefore, the response to X-ray absorption and refractive index in this process are investigated, and the solid target selection model is developed. This model is used to analyze the influence of solid target type and thickness in diagnosis, while avoiding situations where the sample is too hot due to a lot X-ray absorption. Moreover, the influence of hard X-ray on sample temperature at high frequency is considered, and the samples suitable for different X-ray bands are given. The chirped pulse modulation in spectral coding is analyzed, and the influence of dispersion medium and pulse parameters on the diagnostic resolution of spectral coding are obtained. Finally, the error effects of X-ray, spatial coding and spectral coding on the results are analyzed, and the analysis methods and consideration factors of the two coding methods are given. This work is of great significance in using the XFEL pulse arrival time diagnostic device.

A magnetically controlled chemical-mechanical polishing (MC-CMP) approach for fabricating channel-cut silicon crystal optics for the High Energy Photon Source.

Crystal monochromators are indispensable optical components for the majority of beamlines at synchrotron radiation facilities. Channel-cut monochromators are sometimes chosen to filter monochromatic X-ray beams by virtue of their ultrahigh angular stability. Nevertheless, high-accuracy polishing on the inner diffracting surfaces remains challenging, thus hampering their performance in preserving the coherence or wavefront of the photon beam. Herein, a magnetically controlled chemical-mechanical polishing (MC-CMP) approach has been successfully developed for fine polishing of the inner surfaces of channel-cut crystals. This MC-CMP process relieves the constraints of narrow working space dictated by small offset requirements and achieves near-perfect polishing on the surface of the crystals. Using this method, a high-quality surface with roughness of 0.614 nm (root mean square, r.m.s.) is obtained in a channel-cut crystal with 7 mm gap designed for beamlines at the High Energy Photon Source, a fourth-generation synchrotron radiation source under construction. On-line X-ray topography and rocking-curve measurements indicate that the stress residual layer on the crystal surface was removed. Firstly, the measured rocking-curve width is in good agreement with the theoretical value. Secondly, the peak reflectivity is very close to theoretical values. Thirdly, topographic images of the optics after polishing were uniform without any speckle or scratches. Only a nearly 2.5 nm-thick SiO2 layer was observed on the perfect crystalline matrix from high-resolution transmission electron microscopy photographs, indicating that the structure of the bulk material is defect- and dislocation-free. Future development of MC-CMP is promising for fabricating wavefront-preserving and ultra-stable channel-cut monochromators, which are crucial to exploit the merits of fourth-generation synchrotron radiation sources or hard X-ray free-electron lasers.

The MING proposal at SHINE: megahertz cavity enhanced X-ray generation

The cavity-based X-ray free-electron laser (XFEL) has promise in producing fully coherent pulses with a bandwidth of a few meV and very stable intensity, whereas the currently existing self-amplified spontaneous emission (SASE) XFEL is capable of generating ultra-short pulses with chaotic spectra. In general, a cavity-based XFEL can provide a spectral brightness three orders of magnitude higher than that of the SASE mode, thereby opening a new door for cutting-edge scientific research. With the development of superconducting MHz repetition-rate XFEL facilities such as FLASH, European-XFEL, LCLS-II, and SHINE, practical cavity-based XFEL operations are becoming increasingly achievable. In this study, megahertz cavity enhanced X-ray generation (MING) is proposed based on China’s first hard XFEL facility - SHINE, which we refer to as MING@SHINE.

14th International Conference on Synchrotron Radiation Instrumentation (SRI 2021), 28 March to 1 April 2022

The International Conference on Synchrotron Radiation Instrumentation (SRI) is a unique and significant international forum held every three years in the community of synchrotron radiation (SR) and free electron lasers (FEL). It is the prime forum for fostering connections between cutting-edge synchrotron radiation instrumentation, science, and the requirements of the user community. The SRI 2021 had originally been scheduled to take place in Hamburg in summer 2021. Due to the COVID-19 pandemic, it was postponed to 2022 and held as an online event.More than 1160 international participants from 25 countries met virtually at the SRI 2021. In nearly 290 talks and 450 posters, latest results were presented. Although it was an online-only conference, lively discussions took place in the nearly 40 parallel sessions, and the eight poster sessions were also very well attended.The main topics of the SRI conference were: new SR and FEL facilities, update plans of these facilities, and recent developments in various instrumentation areas like beamline design, X-ray optics, sample environments, detectors and spectrometers, data acquisition, and data analysis techniques or automation. These innovations contributed to new results for a wide range of experimental techniques and scientific applications such as X-ray scattering and spectroscopy, bio- and scanning imaging, structural biology crystallography, coherent techniques, or in-situ/operando methods. A dedicated session concerned industrial applications of synchrotron radiation.The field of synchrotron radiation instrumentation is currently seeing very active development due to various factors. Firstly, the number of SR sources world-wide is increasing significantly, with new sources in particular in Europe and in Asia. Secondly, a new generation of storage rings with new multi-bend achromat lattices are being implemented at a growing number of existing facilities. These facilities offer a significant increase of brilliance and coherence and thereby lead to new and improved applications of synchrotron radiation, in particular in the areas of imaging and high spatial resolution. Thirdly, the increase of soft and hard X-ray FEL sources worldwide and the maturation of their experimental techniques and scientific applications is the background for a strongly increasing number of developments for ultrafast time-resolved investigations of dynamic behaviour of materials and reactions. Most of the keynote speakers and many invited and contributed talks or posters at the conference showed new results directly related to these three major developments.Lists of International Advisory Committee (listed by facility), Scientific Programme Committee (listed by facility), Local Organising Committee (listed by facility) are available in this PDF.

Femtosecond-Terawatt Hard X-Ray Pulse Generation with Chirped Pulse Amplification on a Free Electron Laser.

Advances of high intensity lasers have opened up the field of strong field physics and led to a broad range of technological applications. Recent x-ray laser sources and optics development makes it possible to obtain extremely high intensity and brightness at x-ray wavelengths. In this Letter, we present a system design that implements chirped pulse amplification for hard x-ray free electron lasers. Numerical modeling with realistic experimental parameters shows that near-transform-limit single-femtosecond hard x-ray laser pulses with peak power exceeding 1TW and brightness exceeding 4×10^{35} s^{-1} mm^{-2} mrad^{-2}0.1% bandwdith^{-1} can be consistently generated. Realization of such beam qualities is essential for establishing systematic and quantitative understanding of strong field x-ray physics and nonlinear x-ray optics phenomena.

Towards performing high-resolution inelastic X-ray scattering measurements at hard X-ray free-electron lasers coupled with energetic laser drivers.

High-resolution inelastic X-ray scattering is an established technique in the synchrotron community, used to investigate collective low-frequency responses of materials. When fielded at hard X-ray free-electron lasers (XFELs) and combined with high-intensity laser drivers, it becomes a promising technique for investigating matter at high temperatures and high pressures. This technique gives access to important thermodynamic properties of matter at extreme conditions, such as temperature, material sound speed, and viscosity. The successful realization of this method requires the acquisition of many identical laser-pump/X-ray-probe shots, allowing the collection of a sufficient number of photons necessary to perform quantitative analyses. Here, a 2.5-fold improvement in the energy resolution of the instrument relative to previous works at the Matter in Extreme Conditions (MEC) endstation, Linac Coherent Light Source (LCLS), and the High Energy Density (HED) instrument, European XFEL, is presented. Some aspects of the experimental design that are essential for improving the number of photons detected in each X-ray shot, making such measurements feasible, are discussed. A careful choice of the energy resolution, the X-ray beam mode provided by the XFEL, and the position of the analysers used in such experiments can provide a more than ten-fold improvement in the photometrics. The discussion is supported by experimental data on 10 µm-thick iron and 50 nm-thick gold samples collected at the MEC endstation at the LCLS, and by complementary ray-tracing simulations coupled with thermal diffuse scattering calculations.

A multi-million image Serial Femtosecond Crystallography dataset collected at the European XFEL

Serial femtosecond crystallography is a rapidly developing method for determining the structure of biomolecules for samples which have proven challenging with conventional X-ray crystallography, such as for membrane proteins and microcrystals, or for time-resolved studies. The European XFEL, the first high repetition rate hard X-ray free electron laser, provides the ability to record diffraction data at more than an order of magnitude faster than previously achievable, putting increased demand on sample delivery and data processing. This work describes a publicly available serial femtosecond crystallography dataset collected at the SPB/SFX instrument at the European XFEL. This dataset contains information suitable for algorithmic development for detector calibration, image classification and structure determination, as well as testing and training for future users of the European XFEL and other XFELs.

Electrons and X-rays to Muon Pairs (EXMP)

One of the challenges of future muon colliders involves the production of muon beams carrying high phase space densities. In particular, the muon beam normalised transverse emittance is a relevant figure of merit used to meet luminosity requests. A typical issue impacting the achieved transverse emittance in muon collider schemes, thus far considered, is the phase space dilution caused by the Coulomb interaction of primary particles propagating into the target where muons were generated. In this study, we present a new scheme(named electrons and X-rays to muon pairs) for muon beam generation occurring in a vacuum via interactions of electron and photon beams. Setting the center of mass energy at about twice the threshold (i.e., around 350 MeV), the normalised emittance of the muon beam generated via muon pair production reaction (e−+γ→e−+μ++μ−) is largely independent on the emittance of the colliding electron beam and is set basically by the excess of transverse momentum in the muon pair creation. In absence of any other mechanism for emittance dilution, the resulting muon beam, with energy in the range of a few tens of GeV, is characterised by an ultra-low normalised transverse RMS emittance of a few nm rad, corresponding to a geometrical emittance below 10 π pm rad. This opens up the way to a new muon collider paradigm based on muon sources conceived with primary colliding beams delivered by 100 GeV-class energy recovery LINACs interacting with hard-X ray free electron lasers. The challenge is to achieve the requested luminosity of the muon collider adopting a strategy of low muon fluxes/currents combined to ultra-low emittances, to largely reduce the levels of muon beam-induced backgrounds.

Single-exposure X-ray phase imaging microscopy with a grating interferometer.

The advent of hard X-ray free-electron lasers enables nanoscopic X-ray imaging with sub-picosecond temporal resolution. X-ray grating interferometry offers a phase-sensitive full-field imaging technique where the phase retrieval can be carried out from a single exposure alone. Thus, the method is attractive for imaging applications at X-ray free-electron lasers where intrinsic pulse-to-pulse fluctuations pose a major challenge. In this work, the single-exposure phase imaging capabilities of grating interferometry are characterized by an implementation at the I13-1 beamline of Diamond Light Source (Oxfordshire, UK). For comparison purposes, propagation-based phase contrast imaging was also performed at the same instrument. The characterization is carried out in terms of the quantitativeness and the contrast-to-noise ratio of the phase reconstructions as well as via the achievable spatial resolution. By using a statistical image reconstruction scheme, previous limitations of grating interferometry regarding the spatial resolution can be mitigated as well as the experimental applicability of the technique.

Design of a Hybrid Split-Delay Line for Hard X-ray Free-Electron Lasers

High repetition-rate X-ray free-electron lasers (XFELs) enable the study of fast dynamics on microsecond time scales. Split-delay lines (SDLs) further bring the time scale down to femtoseconds by splitting and delaying the XFEL pulses. Crystals and multilayers are two common types of optical elements in SDLs, offering either long delay ranges or high temporal accuracy. In this work, we introduce the design of a hybrid SDL for the coherent diffraction endstation of Shanghai High Repetition Rate XFEL and Extreme Light Facility (SHINE). It uses crystals for the first branch and multilayers for the second one, thus simultaneously offering a relatively long delay range and high temporal accuracy. Moreover, a third branch can be installed to switch the SDL to the all-crystal configuration for longer delay ranges.

Single-shot experiments at the soft X-FEL FERMI using a back-side-illuminated scientific CMOS detector.

The latest Complementary Metal Oxide Semiconductor (CMOS) 2D sensors now rival the performance of state-of-the-art photon detectors for optical application, combining a high-frame-rate speed with a wide dynamic range. While the advent of high-repetition-rate hard X-ray free-electron lasers (FELs) has boosted the development of complex large-area fast CCD detectors in the extreme ultraviolet (EUV) and soft X-ray domains, scientists lacked such high-performance 2D detectors, principally due to the very poor efficiency limited by the sensor processing. Recently, a new generation of large back-side-illuminated scientific CMOS sensors (CMOS-BSI) has been developed and commercialized. One of these cost-efficient and competitive sensors, the GSENSE400BSI, has been implemented and characterized, and the proof of concept has been carried out at a synchrotron or laser-based X-ray source. In this article, we explore the feasibility of single-shot ultra-fast experiments at FEL sources operating in theEUV/soft X-ray regime with an AXIS-SXR camera equipped with the GSENSE400BSI-TVISB sensor. We illustrate the detector capabilities by performing a soft X-ray magnetic scattering experiment at the DiProi end-station of the FERMI FEL. These measurements show the possibility of integrating this camera for collecting single-shot images at the 50 Hz operation mode of FERMI with a cropped image size of 700× 700 pixels. The efficiency of the sensor at a working photon energy of 58 eV and the linearity over the large FEL intensity have been verified. Moreover, on-the-fly time-resolved single-shot X-ray resonant magnetic scattering imaging from prototype Co/Pt multilayer films has been carried out with a time collection gain of 30 compared to the classical start-and-stop acquisition method performed with the conventional CCD-BSI detector available at the end-station.