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A Nanobeam X‐ray Experiments (NXE) instrument was developed and installed at the hard X‐ray beamline of the Pohang Accelerator Laboratory X‐ray Free Electron Laser. This instrument consists of a diagnostic system, focusing optics, an X‐ray diffraction endstation and a femtosecond laser delivery system. The NXE instrument enables sophisticated X‐ray experiments using nanofocused X‐rays. At a 9.5 keV X‐ray energy, the beam was successfully focused to 390 nm × 230 nm at the focal plane using Kirkpatrick–Baez mirrors. Following the successful commissioning experiments in December 2021 and April 2022, the instrument became available for regular user experiments in January 2023. The first user experiment was conducted in January 2024. This article provides detailed information on the beamline optics, the NXE instrument, and its performance and capabilities. The Nanobeam X‐ray Experiments (NXE) instrument at the Pohang Accelerator Laboratory X‐ray Free Electron Laser (PAL‐XFEL) is introduced. The NXE instrument enables users to conduct X‐ray experiments with nanofocused X‐rays.

Characterizing the properties of X‐ray free‐electron laser (XFEL) sources is a critical step for optimization of performance and experiment planning. The recent availability of MHz XFELs has opened up a range of new opportunities for novel experiments but also highlighted the need for systematic measurements of the source properties. Here, MHz‐enabled beam imaging diagnostics developed for the SPB/SFX instrument at the European XFEL are exploited to measure the shot‐to‐shot intensity statistics of X‐ray pulses. The ability to record pulse‐integrated two‐dimensional transverse intensity measurements at multiple planes along an XFEL beamline at MHz rates yields an improved understanding of the shot‐to‐shot photon beam intensity variations. These variations can play a critical role, for example, in determining the outcome of single‐particle imaging experiments and other experiments that are sensitive to the transverse profile of the incident beam. It is observed that shot‐to‐shot variations in the statistical properties of a recorded ensemble of radiant intensity distributions are sensitive to changes in electron beam current density. These changes typically occur during pulse‐distribution to the instrument and are currently not accounted for by the existing suite of imaging diagnostics. Modulations of the electron beam orbit in the accelerator are observed to induce a time‐dependence in the statistics of individual pulses – this is demonstrated by applying radio‐frequency trajectory tilts to electron bunch‐trains delivered to the instrument. We discuss how these modifications of the beam trajectory might be used to modify the statistical properties of the source and potential future applications. Systematic fluctuations in the pulse–pulse intensity profile of a MHz X‐ray free‐electron laser (FEL) source have been observed that are not described by fundamental FEL theory. The sensitivity of these fluctuations to modifications of the electron‐beam orbit in the accelerator is demonstrated as a potential route to beam optimization.

Aqueous iron (III) oxide nanoparticles were irradiated with pure self-amplified spontaneous emission (SASE) X-ray free-electron laser (XFEL) pulses tuned to the energy around the Fe K-edge ionization threshold. For each XFEL shot, the incident X-ray pulse spectrum and Fe Kβ emission spectrum were measured synchronously with dedicated spectrometers and processed through a reconstruction algorithm allowing for the determination of Fe Kβ resonant X-ray emission spectroscopy (RXES) plane with high energy resolution. The influence of the number of X-ray shots employed in the experiment on the reconstructed data quality was evaluated, enabling the determination of thresholds for good data acquisition and experimental times essential for practical usage of scarce XFEL beam times.

A transmissive single-shot spectrometer has been developed to monitor shot-to-shot spectral structures in the hard X-ray beamline of the Pohang Accelerator Laboratory X-ray Free Electron Laser (PAL-XFEL). The established spectrometer comprises 10 µm-thick Si crystals bent to a radius of curvature of 100 mm. Depending on the photon energy range, either the Si (111) or Si (110) crystal can be selected for spectral analysis. Especially in the energy range 4.5–17 keV, the spectrometer is designed to cover a spectral range wider than the full free-electron laser bandwidth and to guarantee a high resolution sufficient for resolving each spectral spike. This paper presents the design specifications, instruments and performance of this spectrometer, which has also been applied to demonstrate the spectral properties of various XFEL sources, such as self-amplified spontaneous emission, monochromatic and seeded beams.

Crystallization is a fundamental natural phenomenon and the ubiquitous physical process in materials science for the design of new materials. So far, experimental observations of the structural dynamics in crystallization have been mostly restricted to slow dynamics. We present here an exclusive way to explore the dynamics of crystallization in highly controlled conditions (i.e., in the absence of impurities acting as seeds of the crystallites) as it occurs in vacuum. We have measured the early formation stage of solid Xe nanoparticles nucleated in an expanding supercooled Xe jet by means of an X-ray diffraction experiment with 10-fs X-ray free-electron laser (XFEL) pulses. We found that the structure of Xe nanoparticles is not pure face-centered cubic (fcc), the expected stable phase, but a mixture of fcc and randomly stacked hexagonal close-packed (rhcp) structures. Furthermore, we identified the instantaneous coexistence of the comparably sized fcc and rhcp domains in single Xe nanoparticles. The observations are explained by the scenario of structural aging, in which the nanoparticles initially crystallize in the highly stacking-disordered rhcp phase and the structure later forms the stable fcc phase. The results are reminiscent of analogous observations in hard-sphere systems, indicating the universal role of the stacking-disordered phase in nucleation.

AbstractInorganic–organic hybrid materials represent a large share of newly reported structures, owing to their simple synthetic routes and customizable properties1. This proliferation has led to a characterization bottleneck: many hybrid materials are obligate microcrystals with low symmetry and severe radiation sensitivity, interfering with the standard techniques of single-crystal X-ray diffraction2,3 and electron microdiffraction4–11. Here we demonstrate small-molecule serial femtosecond X-ray crystallography (smSFX) for the determination of material crystal structures from microcrystals. We subjected microcrystalline suspensions to X-ray free-electron laser radiation12,13 and obtained thousands of randomly oriented diffraction patterns. We determined unit cells by aggregating spot-finding results into high-resolution powder diffractograms. After indexing the sparse serial patterns by a graph theory approach14, the resulting datasets can be solved and refined using standard tools for single-crystal diffraction data15–17. We describe the ab initio structure solutions of mithrene (AgSePh)18–20, thiorene (AgSPh) and tethrene (AgTePh), of which the latter two were previously unknown structures. In thiorene, we identify a geometric change in the silver–silver bonding network that is linked to its divergent optoelectronic properties20. We demonstrate that smSFX can be applied as a general technique for structure determination of beam-sensitive microcrystalline materials at near-ambient temperature and pressure.

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. High‐resolution inelastic X‐ray scattering measurements at hard X‐ray free‐electron lasers coupled with energetic laser drivers have shown a 2.5‐fold improved energy resolution compared with previous experiments at similar XFEL instruments. Aspects of the experimental design that can be adjusted to improve the number of recorded photons on the detector are discussed.

The existence of charge-density-wave (CDW) correlations in cuprate superconductors has now been established. However, the nature of the CDW ground state has remained uncertain because disorder and the presence of superconductivity typically limit the CDW correlation lengths to only a dozen unit cells or less. Here we explore the field-induced 3D CDW correlations in extremely pure detwinned crystals of YBa₂Cu₃Oₓ (YBCO) ortho-II and ortho-VIII at magnetic fields in excess of the resistive upper critical field (H c2) where superconductivity is heavily suppressed. We observe that the 3D CDW is unidirectional and possesses a long in-plane correlation length as well as significant correlations between neighboring CuO₂ planes. It is significant that we observe only a single sharply defined transition at a critical field proportional to H c2, given that the field range used in this investigation overlaps with other high-field experiments including quantum oscillation measurements. The correlation volume is at least two to three orders of magnitude larger than that of the zero-field CDW. This is by far the largest CDW correlation volume observed in any cuprate crystal and so is presumably representative of the high-field ground state of an “ideal” disorder-free cuprate.

The dynamics of thin magnetic films revealed by ultrafast laser techniques cannot be explained by standard equilibrium descriptions. Diffraction experiments using an X-ray laser now allow the spin dynamics of the separate magnetic constituents of ferromagnetic GdFeCo alloys to be spatially resolved. Ultrafast laser techniques have revealed extraordinary spin dynamics in magnetic materials 1 , 2 , 3 , 4 , 5 , 6 that equilibrium descriptions of magnetism 7 cannot explain. Particularly important for future applications is understanding non-equilibrium spin dynamics following laser excitation on the nanoscale, yet the limited spatial resolution of optical laser techniques has impeded such nanoscale studies. Here we present ultrafast diffraction experiments with an X-ray laser that probes the nanoscale spin dynamics following optical laser excitation in the ferrimagnetic alloy GdFeCo, which exhibits macroscopic all-optical switching 4 , 8 , 9 . Our study reveals that GdFeCo displays nanoscale chemical and magnetic inhomogeneities that affect the spin dynamics. In particular, we observe Gd spin reversal in Gd-rich nanoregions within the first picosecond driven by the non-local transfer of angular momentum from larger adjacent Fe-rich nanoregions. These results suggest that a magnetic material’s microstructure can be engineered to control transient laser-excited spins, potentially allowing faster (~ 1 ps) spin reversal than in present technologies 10 , 11 , 12 .

X-ray free-electron lasers, with pulse durations ranging from a few to several hundred femtoseconds, are uniquely suited for studying atomic, molecular, chemical and biological systems. Characterizing the temporal profiles of these femtosecond X-ray pulses that vary from shot to shot is not only challenging but also important for data interpretation. Here we report the time-resolved measurements of X-ray free-electron lasers by using an X-band radiofrequency transverse deflector at the Linac Coherent Light Source. We demonstrate this method to be a simple, non-invasive technique with a large dynamic range for single-shot electron and X-ray temporal characterization. A resolution of less than 1 fs root mean square has been achieved for soft X-ray pulses. The lasing evolution along the undulator has been studied with the electron trapping being observed as the X-ray peak power approaches 100 GW. Characterizing femtosecond X-ray pulses that vary from shot to shot is important for data interpretation. Here, Behrens et al. measure time-resolved lasing effects on the electron beam and extract the temporal profile of X-ray pulses using an X-band radiofrequency transverse deflector.