Fourth-generation Synchrotron Research Articles

First X-ray spectral ptychography and resonant ptychographic computed tomography experiments at the SWING beamline from Synchrotron SOLEIL.

X-ray ptychography and ptychographic computed tomography have seen a rapid rise since the advent of fourth-generation synchrotrons with a high degree of coherent radiation. In addition to quantitative multiscale structural analysis, ptychography with spectral capabilities has been developed, allowing for spatial-localized multiscale structural and spectral information of samples. The SWING beamline of Synchrotron SOLEIL has recently developed a nanoprobe setup where the endstation's first spectral and resonant ptychographic measurements have been successfully conducted. A metallic nickel wire sample was measured using 2D spectral ptychography in XANES mode and resonant ptychographic tomography. From the 2D spectral ptychography measurements, the spectra of the components of the sample's complex-valued refractive index, δ and β, were extracted, integrated along the sample thickness. By performing resonance ptychographic tomography at two photon energies, 3D maps of the refractive index decrement, δ, were obtained at the Ni K-edge energy and another energy above the edge. These maps allowed the detection of impurities in the Ni wire. The significance of accounting for the atomic scattering factor is demonstrated in the calculation of electron density near a resonance through the use of the δvalues. These results indicate that at the SWING beamline it is possible to conduct state-of-the-art spectral and resonant ptychography experiments using the nanoprobe setup.

In situ/Operando Synchrotron Radiation Analytical Techniques for CO2/CO Reduction Reaction: From Atomic Scales to Mesoscales.

Electrocatalytic carbon dioxide/carbon monoxide reduction reaction (CO(2)RR) has emerged as a prospective and appealing strategy to realize carbon neutrality for manufacturing sustainable chemical products. Developing highly active electrocatalysts and stable devices has been demonstrated as effective approach to enhance the conversion efficiency of CO(2)RR. In order to rationally design electrocatalysts and devices, a comprehensive understanding of the intrinsic structure evolution within catalysts and micro-environment change around electrode interface, particularly under operation conditions, is indispensable. Synchrotron radiation has been recognized as a versatile characterization platform, garnering widespread attention owing to its high brightness, elevated flux, excellent directivity, strong polarization and exceptional stability. This review systematically introduces the applications of synchrotron radiation technologies classified by radiation sources with varying wavelengths in CO(2)RR. By virtue of in situ/operando synchrotron radiationanalytical techniques, we also summarize relevant dynamic evolution processes from electronic structure, atomic configuration, molecular adsorption, crystal lattice and devices, spanning scales from the angstrom to the micrometer. The merits and limitations of diverse synchrotron characterization techniques are summarized, and their applicable scenarios in CO(2)RR are further presented. On the basis of the state-of-the-art fourth-generation synchrotron facilities, a perspective for further deeper understanding of the CO(2)RR process using synchrotron radiation analytical techniques is proposed.

Perspectives for infrared beamlines in fourth-generation synchrotron facilities.

With several fourth-generation, or diffraction-limited, storage rings and multiple beamlines in operation, the missing range of the spectrum was infrared…until recently.

Button-Type Beam Position Monitor Development for Fourth-Generation Synchrotron Light Sources: Numerical Modeling and Test Bench Measurements.

This paper addresses the design of beam position monitor (BPM) devices suitable for fourth-generation diffraction-limited X-ray storage rings. Detailed investigations of the electromagnetic (EM) phenomena occurring inside the component under various working conditions are carried out by considering different BPM EM models defined by their geometry and materials. Moving from a theoretical characterization of the common round geometry, rhomboidal structures are studied through a careful numerical analysis relying on advanced computer-aided tools. Several critical elements, such as wakefields, pick-up signal extraction, and trapped and propagating modes, are explored from the simulation point of view and from the experimental one, by deploying a manufactured microwave test bench, which is employed to measure the radio frequency behavior of a BPM prototype built at Elettra Sincrotrone Trieste. The aim of the proposed study is to identify a satisfactory tradeoff between achievable performance and practical realizability for BPM devices operating in last-generation light sources.

Synchrotron infrared nanospectroscopy in fourth-generation storage rings.

Fourth-generation synchrotron storage rings represent a significant milestone in synchrotron technology, offering outstandingly bright and tightly focused X-ray beams for a wide range of scientific applications. However, due to their inherently tight magnetic lattices, these storage rings have posed critical challenges for accessing lower-energy radiation, such as infrared (IR) and THz. Here the first-ever IR beamline to be installed and to operate at a fourth-generation synchrotron storage ring is introduced. This work encompasses several notable advancements, including a thorough examination of the new IR source at Sirius, a detailed description of the radiation extraction scheme, and the successful validation of our optical concept through both measurements and simulations. This optimal optical setup has enabled us to achieve an exceptionally wide frequency range for our nanospectroscopy experiments. Through the utilization of synchrotron IR nanospectroscopy on biological and hard matter samples, the practicality and effectiveness of this beamline has been successfully demonstrated. The advantages of fourth-generation synchrotron IR sources, which can now operate with unparalleled stability as a result of the stringent requirements for producing low-emittance X-rays, are emphasized.

Imaging extended single crystal lattice distortion fields with multi-peak Bragg ptychography

Imaging extended single crystal lattice distortion fields with multi-peak Bragg ptychography

High-pressure X-ray photon correlation spectroscopy at fourth-generation synchrotron sources.

A new experimental setup combining X-ray photon correlation spectroscopy (XPCS) in the hard X-ray regime and a high-pressure sample environment has been developed to monitor the pressure dependence of the internal motion of complex systems down to the atomic scale in the multi-gigapascal range, from room temperature to 600 K. The high flux of coherent high-energy X-rays at fourth-generation synchrotron sources solves the problems caused by the absorption of diamond anvil cells used to generate high pressure, enabling the measurement of the intermediate scattering function over six orders of magnitude in time, from 10-3 s to 103 s. The constraints posed by the high-pressure generation such as the preservation of X-ray coherence, as well as the sample, pressure and temperature stability, are discussed, and the feasibility of high-pressure XPCS is demonstrated through results obtained on metallic glasses.

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

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

Site-vibration assessment for the SKIF SYNCHROTRON

The Siberian ring source of photons (SKIF) is a new fourth-generation synchrotron light source currently under construction in Koltsovo city, Russia. The beam stability of modern synchrotron sources, characterized by low emittance, is sensitive to insignificant levels of ground vibrations. We assessed the seismic noise variation from external sources recorded at the construction site of the SKIF. For the frequency range 1–20 Hz, the transmission coefficients for the vertical and horizontal recording components were 0.38 and 0.725, respectively. In the frequency range 20–100 Hz – 0.12 and 0.06, respectively. Analysis of experimental data shows the effectiveness of suppressing high-amplitude external noise in the frequency range of 2-100 Hz when transmitting vibrations from the ground to the SKIF storage ring basement. The coefficients determined for the basement match well with the design model.

FDIP—A Fast Diffraction Image Processing Library for X-ray Crystallography Experiments

Serial crystallography (SX) is a cutting-edge technique in structural biology, involving the systematic collection of X-ray diffraction data from numerous randomly oriented microcrystals. To extract comprehensive three-dimensional information about the studied system, SX utilises thousands of measured diffraction patterns. As such, SX takes advantages of the properties of modern X-ray sources, including Free Electron Lasers (FELs) and third and fourth generation synchrotrons, as well as contemporary high-repetition-rate detectors. Efficient analysis of the extensive datasets generated during SX experiments demands fast and effective algorithms. The FDIP library offers meticulously optimised functions tailored for preprocessing data obtained in SX experiments. This encompasses tasks such as background subtraction, identification and masking of parasitic streaks, elimination of unwanted powder diffraction (e.g., from ice or salt crystals), and pinpointing useful Bragg peaks in each diffraction pattern. The library is equipped with a user-friendly graphical interface for facile parameter adjustment tailored to specific datasets. Compatible with popular SX processing software like OnDA, Cheetah, CrystFEL, and Merge3D, the FDIP library enhances the capabilities of these tools for streamlined and precise serial crystallography analyses.

Single-photon counting detectors for diffraction-limited light sources

When first introduced, single-photon counting detectors reshaped crystallography at synchrotrons. Their fast readout speed enabled, for example, shutter-less data collection and fine slicing of the rotation angle and boosted the development of new experimental techniques like ptychography. Under optimal conditions, single-photon counting detectors provide an unlimited dynamic range with image noise only limited by the Poisson statistics of the incoming photons. Counting the pulses from individual photons, essentially what made the detectors so successful, also causes the main drawback, which is the loss of efficiency at high photon fluxes due to pulse pileup in the analog front end. To fully take advantage of diffraction-limited light sources, the next-generation single-photon counters need to improve their count rate capabilities in the same order of magnitude as the increased flux. Moreover, fast frame rates (a few kHz) are required to cope with the shorter dwell time achievable, thanks to the higher flux. Detector architecture with multiple comparators and counters can open new possibilities for energy-resolved imaging, while interpixel communication can overcome the issues arising from charge sharing and reduce the loss of efficiency at the pixel corners. Coupling single-photon counting detectors to high-Z sensors for hard X-ray detection (>20 keV) and to low-gain avalanche diodes (LGADs) for soft X-rays is also necessary to make use of the increased coherence of the new light sources over the full radiation spectrum. In this paper, we present possible strategies to improve the performance of single-photon counting detectors at the fourth-generation synchrotron sources and compare them to charge integrating detectors.

Heitt Mjölnir: a heated miniature triaxial apparatus for 4D synchrotron microtomography.

Third- and fourth-generation synchrotron light sources with high fluxes and beam energies enable the use of innovative X-ray translucent experimental apparatus. These experimental devices access geologically relevant conditions whilst enabling in situ characterization using the spatial and temporal resolutions accessible at imaging beamlines. Here, Heitt Mjölnir is introduced, a heated miniature triaxial rig based on the design of Mjölnir, but covering a wider temperature range and larger sample volume at similar pressure capacities. This device is designed to investigate coupled thermal, chemical, hydraulic and mechanical processes from grain to centimetre scales using cylindrical samples of 10 mm × 20 mm (diameter × length). Heitt Mjölnir can simultaneously reach confining (hydraulic) pressures of 30 MPa and 500 MPa of axial stress with independently controlled sample pore fluid pressure < 30 MPa. This internally heated apparatus operates to temperatures up to 573 K with a minimal vertical thermal gradient in the sample of <0.3 K mm-1. This new apparatus has been deployed in operando studies at the TOMCAT (Swiss Light Source), I12 JEEP (Diamond Light Source) and PSICHÉ (Synchrotron SOLEIL) beamlines for 4D X-ray microtomography with scan intervals of a few minutes. Heitt Mjölnir is portable and modular, allowing a wide range of 4D characterizations of low-grade metamorphism and deformational processes. It enables spatially and temporally resolved fluid-rock interaction studies at conditions of crustal reservoirs and is suitable for characterization of material properties in geothermal, carbonation or subsurface gas storage applications. Technical drawings and an operation guide are included in this publication.

Obtaining picosecond x-ray pulses from fourth generation synchrotron light sources

Obtaining picosecond x-ray pulses from fourth generation synchrotron light sources

A study of performance comparison of databases for HALF data archiving system

The Hefei Advanced Light Facility (HALF) is a 2.2 GeV fourth-generation synchrotron radiation light source. The HALF control system is a distributed control system based on Experimental Physics and Industrial Control System (EPICS). As the essential part of the HALF control system, the Historical Data Archiving System (HDAS) is responsible to store operational data for the entire facility including the accelerator and beamlines, and provides the functions for data query and analysis. According to the estimation based on the HALF scale, approximately 25,000 EPICS PVs will be stored in HDAS, and these accumulated massive data require a dedicated database for persistent storage and management. Under the EPICS PV data scenario of HALF, a fair database test platform is designed and built to test the read-write performance of databases commonly used in the particle accelerator field. The tested objects include EPICS Archiver Appliance and the five databases MongoDB, HBase, InfluxDB, TimescaleDB, and Cassandra. Additionally, research on the five databases software ecosystem is conducted for the development and extension of HDAS. The test results indicate that TimescaleDB has the fastest read performance, and 1.4×10^6 items of data can be read per second. TimescaleDB also has superior write performance. 1.2 × 105 items of data can be written per second, which can fully meet the writing requirements of HDAS. Regarding the software ecosystem, TimescaleDB is compatible with a larger number of data visualization software and big data processing frameworks. Therefore, TimescaleDB is more suitable as the HDAS database. In the future, a TimescaleDB distributed cluster will be designed and deployed, and an HDAS prototype system will be developed based on this cluster.

A low-frequency normal conducting cavity with higher-order mode damping for fourth-generation synchrotron radiation sources.

The utilization of a low-frequency (<200MHz) RF system in storage facilitates the attainment of ultra-low emittances in synchrotron light sources through on-axis injection. This paper focuses on the development of a low-frequency normal conducting (NC) cavity with higher-order mode (HOM) damping for fourth-generation synchrotron light sources. We propose a novel approach to achieve efficient HOM damping in a NC cavity by optimizing the lowest frequency HOM and implementing a beam-line absorber. Notably, unlike conventional NC cavities, the presence of a large beam tube for the beam-line absorber does not compromise the accelerating performance in a coaxial resonant cavity, enabling effective HOM damping while maintaining a high shunt impedance. Through simulations, the prototype design of a 166.6MHz HOM-damped cavity demonstrates a fundamental mode impedance of ∼8 MΩ, with longitudinal and transverse HOM impedances below 2.0 and 50 kΩ/m, respectively.

Kilohertz serial crystallography with the JUNGFRAU detector at a fourth-generation synchrotron source.

Serial and time-resolved macromolecular crystallography are on the rise. However, beam time at X-ray free-electron lasers is limited and most third-generation synchrotron-based macromolecular crystallography beamlines do not offer the necessary infrastructure yet. Here, a new setup is demonstrated, based on the JUNGFRAU detector and Jungfraujoch data-acquisition system, that enables collection of kilohertz serial crystallography data at fourth-generation synchrotrons. More importantly, it is shown that this setup is capable of collecting multiple-time-point time-resolved protein dynamics at kilohertz rates, allowing the probing of microsecond to second dynamics at synchrotrons in a fraction of the time needed previously. A high-quality complete X-ray dataset was obtained within 1 min from lysozyme microcrystals, and the dynamics of the light-driven sodium-pump membrane protein KR2 with a time resolution of 1 ms could be demonstrated. To make the setup more accessible for researchers, downstream data handling and analysis will be automated to allow on-the-fly spot finding and indexing, as well as data processing.

Two-dimensional spatial coherence measurement of X-ray sources using aperture array mask.

Fourth-generation synchrotron radiation delivers x-ray sources with unprecedented coherence and brilliance, which enables the development of many advanced coherent techniques taking advantage of the inherent high coherence of the x-ray beams. Simple and accurate measurement of two-dimensional (2D) coherence is of utmost importance for the applications of these coherent experimental techniques. Here, we propose a novel approach based on diffraction of aperture array mask (AAM) to obtain accurate 2D spatial coherence with a single-shot measurement. We utilize a coherent mode decomposition algorithm to simulate the diffraction of AAM illuminated by Gaussian-Schell model beam and demonstrate that spatial coherence function of the incident light beam can be accurately and robustly retrieved. We expect that this new approach will be applied into transverse coherence measurements for the new-generation synchrotron radiation source and relevant coherent experimental techniques.

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.

Exploring beam size measurement based on the Talbot effect at BEPCII.

Vertical beam size measurements were carried out at Beijing Electron-Positron Collider II (BEPCII) using a phase grating and an absorption grating based on the Talbot effect. The transverse coherence of synchrotron radiation is closely related to beam size. Due to the partial coherence of the synchrotron radiation source, the coherence length can be calculated by measuring the visibility decay of interferograms recorded at different distances behind the gratings. A vertical beam size of 68.19 ± 2 µm was obtained based on the relationship between the coherence length and beam size at the 3W1 beamline of BEPCII. A comparison of the vertical emittance derived from the grating Talbot method and the synchrotron radiation visible light interferometer method was presented. The vertical emittances from the two methods are 1.41 nm rad and 1.40 nm rad, respectively. The 0.1% difference indicates that the grating Talbot method for beam size measurement is reliable. This technique has great potential for small beam size measurement of fourth-generation synchrotron radiation light sources, considering its small diffraction limitation and simple experimental setups.

The structure of magnesium stearate trihydrate determined from a micrometre-sized single crystal using a microfocused synchrotron X-ray beam.

Crystalline magnesium stearate has been extensively used as an additive in pharmaceutical and other industries for decades. However, the lack of suitably large crystals has hindered the determination of the crystal structure and thereby a more fundamental understanding of the structure-functionality relationship. Presented here is the structure of magnesium stearate trihydrate as determined from X-ray diffraction data of a micrometre-sized single crystal measured at a fourth-generation synchrotron facility. Despite the small size of the single crystals and the weak diffraction, it was possible to determine the positions of the non-hydrogen atoms reliably. Periodic dispersion-corrected density functional theory calculations were used to obtain the positions of the hydrogen atoms playing an important role in the overall organization of the structure via a hydrogen-bond network.