Soft X-ray Free-electron Laser Research Articles

Observation of mammalian living cells with femtosecond single pulse illumination generated by a soft X-ray free electron laser

Soft X-ray transmission microscopy is a powerful tool for visualizing cellular structures due to the natural contrast between organic material and water, but radiation damage has hindered its application to living cells. We have developed a soft X-ray microscope using femtosecond pulse illumination generated by a soft X-ray free electron laser, with which structural change of cells caused by radiation damage is negligible. Employing Wolter mirrors for illumination and objective optics allowed us to perform soft X-ray imaging with a large field of view, enabling observation of mammalian cells. We successfully captured images of living cells in a culture medium visualizing their carbon distribution. The broad wavelength-tunability of soft X-ray free electron lasers, in conjunction with the achromaticity of Wolter mirrors, enabled wavelength resolved cellular imaging.

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.

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.

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.

FURION: modeling of FEL pulses propagation in dispersive soft X-ray beamline systems.

Modern X-ray free-electron lasers (XFELs) can generate pulses with durations ranging from femtoseconds to attoseconds. The numerical evaluation of ultra-short XFEL pulses through beamline systems is a critical process of beamline system design. However, the bandwidth of such ultra-short XFEL pulses is often non-negligible, and the propagation cannot be simply approximated using the central wavelength, especially in dispersive beamline systems. We developed a numerical model which is called Fourier optics based Ultrashort x-Ray pulse propagatION tool (FURION). This model can not only be used to simulate dispersive beamline systems but also to evaluate non-dispersive beamline systems. The FURION model utilizes Fresnel integral and angular spectrum integral to perform ultra-short XFEL pulse propagation in free space. We also present the method for XFEL pulse propagation through different types of dispersive gratings, which are commonly used in soft X-ray beamline systems. By using FURION, a start-to-end simulation of the FEL-1 beamline system at Shenzhen superconducting soft X-ray free electron laser (S3FEL) is carried out. This model can also be used to evaluate gratings-based spectrometers, beam splitters, pulse compressors, and pulse stretchers. This work provides valuable insights into the start-to-end simulation of X-ray beamline systems.

Numerical studies for EuPRAXIA@SPARC_LAB plasma beam driven working point

The realization of a plasma based user facility on the model of EuPRAXIA@SPARC_LAB requires to design a working point for the operation that allows to get an high accelerating gradient preserving a low emittance and low energy spread of the accelerated beam. Such beam is supposed to pilot a soft x-ray free electron laser with a wavelength of 2-4 nm. In this work several simulation scans are presented, varying at the same time the plasma density and driver-witness separation in order to show that, in a realistic working point for EuPRAXIA@SPARC_LAB, it is possible to find an ideal compromise for a witness with a peak current ¿1kA that allows to preserve the energy spread of the core (80% of the charge) below 0.1%, while maintaining an accelerating gradient inside the plasma module around of 1 GV/m. The study is completed with a parametric analysis with the aim of establishing the stability requirements of the RF working point and the plasma channel in order to preserve the energy jitter at the same level of the energy spread.

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.

Feasibility verification of ultrafast FEL generation experimental scheme based on SXFEL

The photon energy in the soft X-ray range corresponds to the fundamental absorption edges of matter. Ultrashort X-ray pulses can be used to observe the breaking of chemical bonds in biochemical reactions and capture the transfer process of electrons in ultrafast physical phenomena. In this paper, the feasibility of ESASE experiments on Shanghai Soft X-ray Free Electron Laser Facility (SXFEL) is theoretically verified. The results show that the ESASE scheme can produce ultrafast light pulses on the order of attosecond, with a peak power of 450 MW. At the same time, the simulation results in this paper verify the feasibility of chirped enhanced SASE schenme based on SXFEL. The results show that compared with the ESASE scheme, the power of the radiation pulse can be greatly improved by this scheme. A relatively low energy electron beam (1.5 GeV) was used to generate about 40 GW of radiation, and the length of the radiation pulse was significantly shortened.

Enhanced harmonic generation for high-repetition-rate soft x-ray free-electron laser

Externally seeded free-electron lasers are promising for generating intense, stable, and fully coherent soft X-ray pulses. An earlier study demonstrates that high brightness and coherent soft X-ray radiation can be produced based on coherent harmonic generation and superradiant principles, termed high-brightness high-gain harmonic generation (HB-HGHG). However, the seed laser at the ultraviolet region cannot induce sufficient energy modulation at high repetition rates due to state-of-the-art laser system limitations. A recently suggested self-modulation scheme shows that the peak power requirement of a seed laser can be reduced by around one order of magnitude in an HGHG setup. In this paper, we present start-to-end simulation results to estimate the feasibility of the self-modulation-enhanced HB-HGHG scheme.

Design and implementation of timing system for single-shot imaging at Shanghai soft X-ray free-electron laser

X-ray free-electron laser (XFEL) as the novel advanced x-ray light source, has excellent properties, such as ultra-high brightness, ultra-shot pulse duration and full coherence. The development of XFEL provides unprecedented opportunities for ultra-fast and ultra-fine science. The XFEL based experimental methods have been widely applied to the frontier research in physics, chemistry, biology etc. High resolution imaging as one of the most promising methods, can provide a direct view of the microworld. The coherent X-ray diffraction imaging (CDI) is a lensless imaging method. It has a lot of advantages at high resolution and quantitative imaging compared with the traditional lens based X-ray imaging methods. As one of the driving forces to constructing XFEL, it has become one of the most important imaging methods at XFEL facilities. By combing the excellent properties of XFEL and advantages of CDI, the single-shot imaging has been realized, based on the concept of “diffraction before destruction”. With the femtosecond XFEL pulse, structural information of the sample can be captured in a single-shot without multiple measurements or data accumulation. The single-shot imaging can effectively avoid radiation damage and improve the spatial resolution of the images. Shanghai soft X-ray free-electron laser facility (SXFEL) is the first XFEL facility operated at the X-ray wavelength in China. The SXFEL can generate ultra-intense coherent femtosecond X-ray pulses with wavelengths spanning 2-15 nm (80-620 eV). There are two undulator lines and two beamlines. Five endstations were designed and constructed for ultrafast chemistry and physics science, atomic and molecular science and biological imaging. The coherent scattering and imaging (CSI) endstation is the first commissioned endstation at SXFEL and focuses on the high spatiotemporal imaging for nano and micro materials with a single-shot imaging method. To realize the single-shot experiment at XFEL, especially for single-shot imaging, the timing system plays a crucial role to ensure the operation of the equipment in sequence. The timing system is responsible for generating precise and adjustable trigger signals that are used to trigger different devices. These signals can be adjusted according to the specific requirements of the devices being triggered, ensuring that the devices are triggered at the desired moments. In a single-shot experiment, only a single pulse should be transmitted to interact with the sample, and all others must be blocked before the previous single-shot experiment is finished. To carry out the single-shot imaging at CSI endstation, a timing system was designed and commissioned at SXFEL. As the maximum repetition rate of SXFEL is 50Hz, a fast X-ray shutter was applied to select only one XFEL pulse. This paper introduces the design and implement procession of timing for SXFEL single-shot imaging. The timing system implemented with White Rabbit(WR) and digital delay and pulse generator (BNC505). Single-shot imaging is realized by synchronizing the sample scanning stages movement and X-ray shutter to select a single pulse to illuminate the sample. At the same time, the X-ray detector was triggered with the timing system to record the single-shot diffraction pattern. During commissioning, the gold nanodisks with a side length of approximately 300 nm and a thickness of about 30nm were imaged at the CSI endstation as test sample. The nanodisks were uniformly dispersed on Si<sub>3</sub>N<sub>4</sub> membranes for single-shot imaging. Because of the ultra-high peak intensity at the focus spot, the samples and membrane were ionized for each XFEL pulse shot. A raster scan was performed on the membranes with an interval of 50 μm to update the sample. With the timing system and X-ray shutter, single-shot diffraction patterns could be recorded using an X-ray detector. From the image of the Si<sub>3</sub>N<sub>4</sub> membrane after raster scanning, the ionized holes with an interval of 50 μm can be recognized. Finally, phase retrieval was applied to the single-shot diffraction pattern to obtain a real-space image of the sample. The resolution of the reconstructed image was estimated by calculating the phase-retrieval transfer function (PRTF). With a citation of the PRTF curve dropping below 1⁄<i>e</i>, the spatial frequency cutoff was determined to be 22.6μm<sup>-1</sup>, corresponding to a half period resolution of 22.1 nm. The results show that the designed timing system can accurately control the time sequence of the imaging process, meeting the requirement for single-shot imaging within 50Hz at SXFEL.

Recent progress of THz source at the SXFEL

Coherent, wide-tunable frequency and high intensity terahertz (THz) source is under preparation at the Shanghai Soft X-ray free-electron laser facility (SXFEL). The electron bunches modulated by frequency beating light can generate coherent, wide-tunable, high intensity THz radiation from 0.1 to 30 THz through wigglers. The electromagnetic wiggler with peak magnetic field up to 1.75 T is adopted and the parameters of the wiggler are optimized to ensure the generation of strong field THz radiation. Due to the limitation of layout space of the SXFEL, the length of wiggler is limited within 5 meters. By properly increasing the charge of the electron beam, the THz pulse energy can be kept at sub mJ level under the proposed different parameters of the wiggler. In this article, we will present the possible layout of THz source on the SXFEL and the S2E simulation of THz radiation of sub mJ magnitude within the 5-meter wiggler.

Design and first-round commissioning result of the SASE beamline at the Shanghai Soft X-ray FEL facility.

The Shanghai Soft X-ray Free-Electron Laser (SXFEL) is the first X-ray free-electron laser facility in China. The SASE beamline, which consists of a pink-beam branch and a mono-beam branch, is one of the two beamlines in the Phase-I construction. The pink-beam branch opened for users in 2023 after successful first-round beamline commissioning. In this paper, the design of the beamline is presented and the performance of the pink-beam branch is reported. The measured energy-resolving power of the online spectrometer is over 6000 @ 400 eV. The focusing spot size of the pink beam is less than 3 µm in both the horizontal and vertical at the endstation.

Ion emission from warm dense matter produced by irradiation with a soft x-ray free-electron laser

We report on an experiment performed at the FLASH2 free-electron laser (FEL) aimed at producing warm dense matter via soft x-ray isochoric heating. In the experiment, we focus on study of the ions emitted during the soft x-ray ablation process using time-of-flight electron multipliers and a shifted Maxwell–Boltzmann velocity distribution model. We find that most emitted ions are thermal, but that some impurities chemisorbed on the target surface, such as protons, are accelerated by the electrostatic field created in the plasma by escaped electrons. The morphology of the complex crater structure indicates the presence of several ion groups with varying temperatures. We find that the ion sound velocity is controlled by the ion temperature and show how the ion yield depends on the FEL radiation attenuation length in different materials.

Coherent sub-femtosecond soft x-ray free-electron laser pulses with nonlinear compression

We demonstrate the generation of coherent soft x-ray free-electron laser (FEL) pulses with a duration below 1 fs using nonlinear compression with a low-charge electron beam (10 pC). The approach is simple, and it does not require any special hardware, so it can be readily implemented at any x-ray FEL facility. We present temporal and spectral diagnostics confirming the production of single-spike sub-femtosecond pulses for photon energies of 642 and 1111 eV. Our work will be important for ultrafast FEL applications requiring soft x-rays.

Sub-nanometer scale depth patterning on sapphire crystal by femtosecond soft x-ray laser pulse irradiation.

Damage thresholds and structures on a metal aluminum and an aluminum oxide crystal induced by the soft x-ray free electron laser irradiations were evaluated. Distinctive differences in damage thresholds and structures were observed for these materials. On the aluminum oxide crystal surface, in particular, a novel, to the best of our knowledge, surface processing, which we suggest defining as "peeling," was recognized. Surface structures formed by peeling had extremely shallow patterning of sub-nanometer depth. For the newly observed peeling process, we proposed a scission of chemical bond, i.e., binding energy model, in the crystal.

Spatiotemporal response of concave VLS grating to ultra-short X-ray pulses.

In soft X-ray free-electron laser (FEL) beamlines, variable-line-spacing (VLS) gratings are often used as dispersive components of monochromators and spectrometers due to their combined dispersion and focusing properties. X-ray FEL pulses passing through the VLS grating can result in not only transverse focusing but also spatiotemporal coupling effects, such as pulse front tilt, pulse front rotation, and pulse stretching. In this paper, we present a theoretical study of the spatiotemporal response of concave VLS gratings to ultra-short X-ray pulses. The theoretical analysis indicates that the tilt angle of the non-zero diffraction orders varies with the propagation distance, and disappears at the focus, where the focal lengths and pulse stretching differ for different diffraction orders. The model demonstrates the pulse duration after the concave VLS grating is the convolution of the initial pulse duration and the stretching term induced by dispersion, while the beam size at the focus in x dimension is the convolution of the geometric scaling beam size and the dispersion term. This work provides a mathematical explanation for the spatiotemporal response of concave VLS grating to ultra-short X-ray pulses and offers valuable insights into the design of FEL grating monochromators, spectrometers, pulse compressors, and pulse stretchers.

An X-ray free-electron laser with a highly configurable undulator and integrated chicanes for tailored pulse properties

X-ray free-electron lasers (FELs) are state-of-the-art scientific tools capable to study matter on the scale of atomic processes. Since the initial operation of X-ray FELs more than a decade ago, several facilities with upgraded performance have been put in operation. Here we present the first lasing results of Athos, the soft X-ray FEL beamline of SwissFEL at the Paul Scherrer Institute in Switzerland. Athos features an undulator layout based on short APPLE-X modules providing full polarisation control, interleaved with small magnetic chicanes. This versatile configuration allows for many operational modes, giving control over many FEL properties. We show, for example, a 35% reduction of the required undulator length to achieve FEL saturation with respect to standard undulator configurations. We also demonstrate the generation of more powerful pulses than the ones obtained in typical undulators. Athos represents a fundamental step forward in the design of FEL facilities, creating opportunities in FEL-based sciences.

High repetition-rate photoinjector laser system for S3FEL

The photoinjector laser system of Shenzhen Superconducting Soft X-Ray Free Electron Laser (S3FEL) is reported in this paper. This laser system operates at up to 1 MHz and produces more than 50 μJ infrared (IR) laser pulses. With a customized fourth harmonic generation (FHG) module, more than 2 μJ ultraviolet (UV) laser pulses were obtained. The power standard deviations of the IR laser and the UV laser are 0.093% and 0.395% respectively. While the pulse energy standard deviations are 1.087% and 1.746% correspondingly. We implemented the pulse stacking scheme to generate flat-top pulses. With four birefringent uniaxial crystals, the Gaussian pulses were converted to flat-top shape, featuring 10 ps pulse width and 0.5 ps rising and falling edges. A cut-Gaussian transverse profile with very sharp rising and falling edges can be produced after the spatial pulse shaper.

Status and future of the soft X-ray free-electron laser beamline at the SHINE

The Shanghai High repetition rate XFEL and Extreme light facility (SHINE) is under construction and aims at generating X-rays between 0.4 and 25 keV with three FEL beamlines at repetition rates of up to 1 MHz. The soft X-ray FEL beamline, FEL-II, will be ready for commissioning in 2025. It is designed to cover the photon energy from 0.4 to 3 keV, in which the baselines of the FEL operation modes are self-amplified spontaneous emission (SASE), self-seeding, echo-enabled harmonic generation (EEHG), and polarization control. Therefore, a high repetition-rate external seed laser, large period length modulator, soft X-ray monochromator, planar undulator, and elliptically polarized undulator have been adopted in the FEL-II beamline. Several potentials such as an ultra-short pulse mode and a multi-color mode are also foreseeable without significant equipment changes in the follow-up operation. A dual-period undulator design is suggested for the echo-enabled harmonic generation (EEHG) commissioning, and it has great potential to break through the unreachable energy of the fully coherent X-ray in the future. The FEL-II beamline will deliver SASE radiation and fully coherent radiation in all the wavelengths of interest.

High-repetition-rate seeded free-electron laser enhanced by self-modulation

The spectroscopic methods for the ultrafast electronic and structural dynamics of materials require fully coherent extreme ultraviolet and soft X-ray radiation with high-average brightness. Seeded free-electron lasers (FELs) are ideal sources for delivering fully coherent soft X-ray pulses. However, due to state-of-the-art laser system limitations, it is challenging to meet the ultraviolet seed laser’s requirements of sufficient energy modulation and high repetition rates simultaneously. The self-modulation scheme has been proposed and recently demonstrated in a seeded FEL to relax the seed laser requirements. Using numerical simulations, we show that the required seed laser intensity in the self-modulation is ~3 orders of magnitude lower than that in the standard high-gain harmonic generation (HGHG). The harmonic self-modulation can launch a single-stage HGHG FEL lasing at the 30th harmonic of the seed laser. Moreover, the proof-of-principle experimental results confirm that the harmonic self-modulation can still amplify the laser-induced energy modulation. These achievements reveal that the self-modulation can not only remarkably reduce the requirements of the seed laser but also improve the harmonic upconversion efficiency, which paves the way for realizing high-repetition-rate and fully coherent soft X-ray FELs.