X-ray Free Electron Laser Facility Research Articles

A snapshot love story: what serial crystallography has done and will do for us.

Serial crystallography, born from groundbreaking experiments at the Linac Coherent Light Source in 2009, has evolved into a pivotal technique in structural biology. Initially pioneered at X-ray free-electron laser facilities, it has now expanded to synchrotron-radiation facilities globally, with dedicated experimental stations enhancing its accessibility. This review gives an overview of current developments in serial crystallography, emphasizing recent results in time-resolved crystallography, and discussing challenges and shortcomings.

Core-Hole Coherent Spectroscopy in Molecules.

We study the ultrafast dynamics initiated by a coherent superposition of core-excited states of nitrous oxide molecule. Using high-level abinitio methods, we show that the decoherence caused by the electronic decay and the nuclear dynamics is substantially slower than the induced ultrafast quantum beatings, allowing the system to undergo several oscillations before it dephases. We propose a proof-of-concept experiment using the harmonic up-conversion scheme available at x-ray free-electron laser facilities to trace the evolution of the created core-excited-state coherence through a time-resolved x-ray photoelectron spectroscopy.

Ultrahigh resolution x-ray Thomson scattering measurements at the European X-ray Free Electron Laser

Using an ultrahigh resolution (ΔE∼0.1eV) setup to measure electronic features in x-ray Thomson scattering (XRTS) experiments at the European XFEL in Germany, we have studied the collective plasmon excitation in aluminium at ambient conditions, which we can measure very accurately even at low momentum transfers. As a result, we can resolve previously reported discrepancies between time-dependent density functional theory simulations and experimental observations. The demonstrated capability for high-resolution XRTS measurements will be a game changer for the diagnosis of experiments with matter under extreme densities, temperatures, and pressures, and unlock the full potential of state-of-the-art x-ray free electron laser (XFEL) facilities to study planetary interior conditions, to understand inertial confinement fusion applications, and for material science and discovery. Published by the American Physical Society 2024

Excitation signatures of isochorically heated electrons in solids at finite wave number explored from first principles

Ultrafast heating of solids with modern x-ray free electron lasers (XFELs) leads to a unique set of conditions characterized by the simultaneous presence of heated electrons in a cold ionic lattice. In this work, we analyze the effect of electronic heating on the dynamic structure factor (DSF) in bulk aluminum (Al) with a face-centered cubic lattice and in silicon (Si) with a crystal diamond structure using first-principles linear-response time-dependent density functional theory simulations. We find a thermally induced red shift of the collective plasmon excitation in both materials. In addition, we show that the heating of the electrons in Al can lead to the formation of a double-plasmon peak due to the extension of the Landau damping region to smaller wave numbers. Finally, we demonstrate that thermal effects generate a measurable and distinct signature (peak-valley structure) in the DSF of Si at small frequencies. Our simulations indicate a variety of new features in the spectrum of x-ray-driven solids, specifically at finite momentum transfer, which can be probed in upcoming x-ray Thomson scattering experiments at various XFEL facilities. Published by the American Physical Society 2024

Experimental Realization of Auger Decay in the Field of a Positive Elementary Charge.

Auger electron spectroscopy is an omnipresent experimental tool in many fields of fundamental research and applied science. The determination of the kinetic energies of the Auger electrons yields information about the element emitting the electron and its chemical environment at the time of emission. Here, we present an experimental approach to determine Auger spectra for emitter sites in the vicinity of a positive elementary charge based on electron-electron-electron and electron-electron-photon coincidence spectroscopy. We observe a characteristic redshift of the Auger spectrum caused by the Coulomb interaction with the charged environment. Our results are relevant for the interpretation of Auger spectra of extended systems like large molecules, clusters, liquids, and solids, in particular in high-intensity radiation fields which are nowadays routinely available, e.g., at x-ray free-electron laser facilities. The effect has been widely ignored in the literature so far, and some interpretations of Auger spectra from clusters might need to be revisited.

Development of undulator motion control system with redundant protections

The undulator is a key luminous component of the Shanghai high repetition rate x-ray free electron laser and extreme light facility, and the motion control system is an important part of the undulator. The main task of the motion control system is to complete the high precision adjustment of the gap and taper between the upper magnetic pole girder and lower magnetic pole girder, so as to adjust the wavelength of the radiation light. According to the development requirements of the motion control system for the U26 undulator, which is a conventional permanent magnet, this paper proposes a new motion control system with double position feedback closed-loop control, including programmable logic controller (PLC) closed-loop control based on position feedback by a linear absolute encoder (LAE) and driver closed-loop control based on position feedback by a rotary absolute encoder (RAE) of a servo motor. Multiple motion tests of the U26 undulator have shown that the repeatability accuracy of the gap is ±50 nm and the gap drive can reach 0.1 µm step size, the error of which is about ±20 nm according to the feedback of the LAE. The conclusion can be drawn that the motion step size and repeatability accuracy of the motion control system for the U26 undulator are improved by one order of magnitude on the basis of meeting all technical requirements. At the same time, motor torque protection, motor temperature protection, and redundant position protection with RAE can further improve the reliability and safety of the motion control system for the U26 undulator.

Self-enhanced coherent harmonic amplification in seeded free-electron lasers

High-intensity, ultrashort, fully coherent X-ray pulses hold great potential for advancing spectroscopic techniques to unprecedented levels. Here, we propose a novel scheme for generating high-brightness and femtosecond-scale soft X-ray radiation within a seeded free-electron laser (FEL) operating at MHz repetition rates. This scheme relies on the principles of self-modulation and superradiance. A relatively weak energy modulation of the pre-bunched electron beam is significantly amplified by the coherent radiation emitted in the self-modulator. Consequently, a coherent signal at ultra-high harmonics of the seed is achieved, and this signal is further amplified in the subsequent radiator through the fresh bunch and superradiant processes. Based on the parameters of the Shanghai soft X-ray FEL facility, three-dimensional simulations have been performed. The simulation results demonstrate that an electron beam with a laser-induced energy modulation as small as 2.3 times the slice energy spread can generate ultrashort coherent radiation pulses of around 2 GW within the water window spectral range. Moreover, the experimental results demonstrate that self-enhanced coherent energy modulation enables the production of coherent signals up to the 15th harmonic of a 266-nm seed laser. These findings indicate that the proposed scheme promises to generate ultrashort and coherent soft X-ray pulses at MHz repetition rates.

Undulator linear taper control at the European X-Ray Free-Electron Laser facility

Undulator linear taper control at the European X-Ray Free-Electron Laser facility

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.

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.

RF direct sampling and processing electronics for SHINE cavity BPM system

Cavity BPMs are crucial for achieving submicron beam alignment in X-ray Free-Electron Lasers (XFEL), particularly in undulator sections. These monitors typically generate RF signals in the S, C, or X band regions. Due to the limitations of analog-to-digital converter's (ADC) bandwidth and sampling rates, and digital signal processing capabilities, heterodyne and homodyne receivers are often employed to down-convert the RF signal to an intermediate frequency (IF) or baseband (Zero IF) respectively before digital sampling. The digitized signal is then processed by Field Programmable Gate Array (FPGA) to get the beam position and phase information. An RF direct-sampling beam signal processor has been developed using ADCs with a bandwidth of 9 GHz and a sampling rate of 2.6 GSPS, and a powerful system-on-chip FPGA. In addition, a prototype RF module without complex down conversion devices has been designed for the SHINE (Shanghai High Repetition Rate XFEL and Extreme Light Facility) cavity BPM. The processor and the RF module make a novel RF direct sampling and processing cavity BPM electronics for SHINE. This is the first attempt to use direct sampling electronics in the C band cavity BPM system. The analog signal processing chain is greatly simplified compared to the down-conversion structure. The performance of this electronics has been analyzed and evaluated in laboratory. The amplitude relative error is 2.0 × 10-4, surpassing the required accuracy of 1 × 10-3 for cavity BPM systems. The phase error is 14 femtoseconds (fs), which also meets the requirements for an RF Beam Arrival Time Monitor (BAM) system. Additionally, the paper introduces the cavity BPM signal processing algorithms and their implementation in FPGA. The processor can deliver pulse-to-pulse beam position measurement above 1 MHz. The RF direct-sampling electronics represents significant advancements in cavity BPM system, large-scale application can be carried out in accelerator facilities like SHINE.

Thermoelastic effects in Bragg reflectors as a potential bottleneck for XFELs with megahertz repetition rate

Bragg reflectors are essential for beam transport in X-ray free-electron laser (XFEL) facilities. On interaction with Bragg reflectors, a part of the pulse energy will be absorbed, causing the propagation of displacement waves due to rapid thermal expansion. It is suspected that these waves may cause stability problems for XFELs operating with megahertz repetition rates. Here, we experimentally investigate the displacement of a diamond Bragg reflector induced by an optical ultra-violet laser pulse, simulating XFEL pulses with mJ pulse energy, both at room temperature and cryogenic temperatures. Our experiment shows negligible damping of the displacement waves on µs timescales, which could cause disruption for subsequent XFEL pulses. We compare our measurements to a simulation framework based on the assumptions of local thermodynamic equilibrium and classical mechanics, observing reasonable agreement. Our results show that thermoelastic effects are critical for a reliable stability assessment of Bragg reflectors, but are often overlooked.

Design of a Pulse Transformer for X-band Klystron

Future linear accelerators require klystrons with higher radio frequency (RF) to drive higher gradient accelerating structure. An x-band accelerator structure was used to accelerate electrons at the Shanghai Soft X-ray Free Electron Laser Facility (SXFEL) in Shanghai Advanced Research Institute, Chinese Academy of Sciences (SARI-CAS). A pulse transformer is a crucial device in an RF system. This study presents a high-voltage pulse transformer used for a 50 MW x-band pulsed klystron in SXFEL. Typical specifications of the pulse transformer are peak pulse voltage 420 kV, peak pulse current 300 A, 50 Hz repetition rate and 1.5 μs flat-top pulse width. Design and optimization of pulse transformer are achieved by using equivalent circuit analytic methods and computational aided simulation. The relevant experiments show that this pulse transformer can meet the requirements of 50MW x-band klystron.

The Pixel Anomaly Detection Tool: a user-friendly GUI for classifying detector frames using machine-learning approaches.

Data collection at X-ray free electron lasers has particular experimental challenges, such as continuous sample delivery or the use of novel ultrafast high-dynamic-range gain-switching X-ray detectors. This can result in a multitude of data artefacts, which can be detrimental to accurately determining structure-factor amplitudes for serial crystallography or single-particle imaging experiments. Here, a new data-classification tool is reported that offers a variety of machine-learning algorithms to sort data trained either on manual data sorting by the user or by profile fitting the intensity distribution on the detector based on the experiment. This is integrated into an easy-to-use graphical user interface, specifically designed to support the detectors, file formats and software available at most X-ray free electron laser facilities. The highly modular design makes the tool easily expandable to comply with other X-ray sources and detectors, and the supervised learning approach enables even the novice user to sort data containing unwanted artefacts or perform routine data-analysis tasks such as hit finding during an experiment, without needing to write code.

High-resolution multi-mode electron and ion imaging spectrometer at SXFEL

A new multi-mode electron and ion (MEI) imaging spectrometer with two arms of VMI and COLTRIMS/VMI (velocity map imaging/cold-target recoil-ion momentum spectroscopy) is designed to combine various photoelectron and ion detection modes for experiments at Shanghai soft x-ray free-electron laser (SXFEL) facility. The experiments can be optionally operated either with both ion and electron detection in a coincidence/covariance manner (VMI arm and COLTRIMS/VMI arm), or only photoelectron/photoion is detected with the high-resolution VMI arm. The simulated resolutions for 30–150 eV photoelectrons and 3.3 eV–18.0 eV N+ and N2+ photoions are up to 1.0% and 3.1%–1.0% according to our simulation, respectively. MEI spectrometer is expected to improve the experimental abilities significantly considering the low-repetition rate of the SXFEL and to enable the investigation of a diverse range of atomic and molecular phenomena triggered by soft x-ray free electron laser irradiation.

Quantum Efficiency Measurement and Modeling of Silicon Sensors Optimized for Soft X-ray Detection

Hybrid pixel detectors have become indispensable at synchrotron and X-ray free-electron laser facilities thanks to their large dynamic range, high frame rate, low noise, and large area. However, at energies below 3 keV, the detector performance is often limited because of the poor quantum efficiency of the sensor and the difficulty in achieving single-photon resolution due to the low signal-to-noise ratio. In this paper, we address the quantum efficiency of silicon sensors by refining the design of the entrance window, mainly by passivating the silicon surface and optimizing the dopant profile of the n+ region. We present the measurement of the quantum efficiency in the soft X-ray energy range for silicon sensors with several process variations in the fabrication of planar sensors with thin entrance windows. The quantum efficiency for 250 eV photons is increased from almost 0.5% for a standard sensor to up to 62% as a consequence of these developments, comparable to the quantum efficiency of backside-illuminated scientific CMOS sensors. Finally, we discuss the influence of the various process parameters on quantum efficiency and present a strategy for further improvement.

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.

Transient responses of double core-holes generation in all-attosecond pump-probe spectroscopy

Double core-holes (DCHs) show remarkable and sensitive effects for understanding electron correlations and coherence. With advanced modulation of x-ray free-electron laser (XFEL) facility, we propose the forthcoming all-attosecond XFEL pump-probe spectroscopy can decipher the hidden photon-initiated dynamics of DCHs. The benchmark case of neon is investigated, and norm-nonconserving Monte-Carlo wavefunction method simulates non-Hermitian dynamics among vast states, which shows superiority in efficiency and reliability. In our scheme, population transfer to DCHs is sequentially irradiated by pump and probe laser. By varying time delay, Stark shifts and quantum path interference of resonant lines sensitively emerge at specific interval of two pulses. These ubiquitous multi-channel effects are also observed in phase-fluctuating pulses, derived from extra phases of impulsive Raman processes by pump laser. Non-perturbation absorption/emission verifies the uniquely interchangeable role of two pules in higher intensity. Our results reveal sensitive and robust responses on pulse parameters, which show potential capacity for XFEL attosecond pulse diagnosis and further attosecond-timescale chemical analysis.

Study and simulation of cryogenic bi-periodic accelerating structure with TM02 mode

To further enhance the accelerating gradient of accelerators, we designed a cryogenic C-band standing wave bi-periodic accelerating structure for the Shanghai Soft X-ray Free Electron Laser Facility (SXFEL). According to the low-temperature environment, material characteristics and technological conditions, the design is completed and it is decided to design the accelerating structure into a bi-periodic magnetic coupling structure. It is a 17-cell structure consisting of 9 accelerating cavities and 8 coupling cavities. To guarantee the symmetry of the field, the structure is doubly-fed. Operating with the π/2 mode standing wave, it is much less sensitive than the standing-wave structure of π-mode. Additionally, the microwave mode is TM02 in coupling cavities that are larger and even less sensitive than the traditional bi-periodic structure. The shape of the coupling cavity can be redesigned to make it tunable.