We report transient highly strained structural states in individual palladium (Pd) nanocrystals, electronically heated using an optical laser, which precede their uniform thermal expansion. Using an X-ray free-electron laser probe, the evolution of individual 111 Bragg peaks is measured as a function of delay time at various laser fluences. Above a laser fluence threshold at a sufficient pump-probe delay, the Bragg peak splits into multiple peaks, indicating heterogeneous strain, before returning to a single peak, corresponding to even heat distribution throughout the lattice expanded crystal. Our findings are supported by a lattice displacement and strain model of a single nanocrystal at different delay times, which agrees with the experimental data. Our observations have implications for understanding femtosecond laser interactions with metals and the potential photo-catalytic performance of Pd.

By laser pump-probe time-resolved coherent magnetic x-ray diffraction imaging, we have measured the migration velocity of antiferromagnetic domain walls in the Mott insulator Sr2IrO4 at 100 K. Coherent diffraction patterns, recorded at the 106 pure-magnetic Bragg peak, showed fringes, which responded distinctly to the excitation laser. These patterns could not be inverted with current phasing algorithms, but could be modeled as four domains with phase shifts consistent with the antiferromagnetic structure. During the laser-induced demagnetization, we observed these domains and their domain walls moving at 3 & times; 106 m/s, significantly faster than acoustic velocities. This is understood to arise from a purely electronic spin contribution to the magnetic structure without any role for coupling to the crystal lattice.

Ultrafast control of lattice motion in metals is a central challenge for high-frequency strain engineering and spintronic applications. Coherent strain control at terahertz (THz) frequencies in metals has remained elusive because free electrons are expected to delocalize energy beyond the optical penetration depth, preventing rapid and efficient stress generation. Here we show that robust and cost-effective metal-metal superlattices (SLs), where periodic repetitions of bilayers - each layer a few atoms thick - are deposited by sputtering, constitute thermoacoustic metamaterials that overcome this limitation. We combine femtosecond X-ray diffraction with mode-resolved density-functional theory and two-temperature modeling to show that electron pressure, rather than phonon stress, drives a large-amplitude coherent terahertz (1 THz) lattice oscillation in sputtered Pt/Cu superlattices. We establish electron pressure as an engineerable, dominant actuation mechanism in metallic metamaterials which can be tailored by the pitch and the constituent materials of the sputtered SL structure, enabling applications such as ultrafast strain-mediated antiferromagnetic spintronic devices.

X-ray Free-Electron Lasers (XFELs) such as the European XFEL (EuXFEL) generate extremely brilliant, ultra-short X-ray pulses at megahertz repetition rates. Because the pulse energy, position, and temporal properties fluctuate strongly from pulse to pulse, precise, non-invasive, pulse-resolved diagnostics are essential for optimal beam delivery and advanced experiments. This work demonstrates the use of electronic-grade single-crystal CVD (scCVD) diamond detectors in a duo-lateral electrode configuration as a high-speed, radiation-hard beam-position monitor and intensity detector for hard X-rays (>20keV), where conventional gas detectors lose efficiency. Two diamond detectors (different thicknesses) were tested at the Materials Imaging and Dynamics (MID) instrument of the EuXFEL. They successfully performed pulse-resolved beam position and intensity measurements at 2.25MHz repetition rate. The position uncertainty was < 1 % of the beam size. Excellent agreement was observed both between the two diamond sensors and with reference detectors (gas ionization chamber and X-ray imager). These results establish duo-lateral scCVD diamond detectors as a powerful, compact, and reliable diagnostic tool for high-repetition-rate hard X-ray FELs, enabling real-time beam-based alignment and intra-pulse-train position feedback.

In this article, we present the experimental protocol and data-processing framework for megahertz X-ray Photon Correlation Spectroscopy (MHz-XPCS) experiments on soft matter samples implemented at the Materials Imaging and Dynamics (MID) instrument of the European X-ray Free-Electron Laser (EuXFEL). Due to the introduction of a standard configuration and the implementation of a highly automated data-processing pipeline, MHz-XPCS measurements can now be conducted and analyzed with minimal user intervention. A key challenge lies in managing the extremely large data volumes generated by the Adaptive Gain Integrating Pixel Detector (AGIPD) - often reaching several petabytes within a single experiment. We describe the technical implementation, discuss the hardware requirements related to effective parallel data processing and propose strategies to enhance data quality, in particular related to data reduction strategies and an improvement of the signal-to-noise ratio. Finally, we address strategies for making the processed data FAIR (Findable, Accessible, Interoperable, Reusable), in alignment with the goals of the DAPHNE4NFDI project.

By combining hard x-ray attosecond pulses from the European XFEL with total-reflection focusing x-ray optics, we generated nanofocused hard x-ray attosecond pulses with intensities and fluences comparable to the highest values attained in the hard x-ray regime. A peak intensity on the order of 10^20 W/cm^2 is confirmed through the observation of saturation in amplified spontaneous emission from copper atoms. These x-ray pulses enable new scientific opportunities, including the exploration of higher-order nonlinear light–matter interactions, damage-free structure determination, and coherent control of atoms and molecules.

Monochromatization and diagnostics of SASE spectral properties over the entire hard X-ray range are important for many experiments utilizing transverse and longitudinal coherence of XFEL beam. For this purpose the Materials Imaging and Dynamics instrument at European XFEL is equipped with two cryo-cooled double-crystal monochromators using Si111 and Si220 optics. Optical parameters, design and performance of both monochromators are presented.

Pair distribution functions from individual femtosecond X-ray pulses have the potential to elucidate the structure of transient states in matter, such as those found in liquid systems. To demonstrate this possibility an experiment was conducted at the Materials Imaging and Dynamics instrument of European X-ray Free Electron Laser Facility. We utilized the large field of view detector configuration, exploiting single high-flux X-ray pulses of femtosecond duration at 23 keV photon energy. After deconvolution from the pattern termination function, we show here pair distribution functions of liquid water at approximately 260 K. These results demonstrate that current X-ray free electron laser methods can acquire pair distribution functions on the femtosecond timescale that have potential to capture transient state of liquids.

Material processing with femtosecond lasers has attracted enormous attention because of its potential for technology and industrial applications. In parallel, time-resolved x-ray diffraction has been successfully used to study ultrafast structural distortion dynamics in semiconductor thin films or surface layers. However, real-world processing applications mostly are concerned with bulk materials, which prevents the use of x-ray surface based techniques. For processing applications, a fast and depth-sensitive probe is needed. To address this, we present a novel technique based on ultrafast x-ray dynamical diffraction (UDD) capable of imaging transient strain distributions inside bulk crystals upon laser excitation. This pump-probe technique provides a complete picture of thetemporal evolution of ultrafast distorted lattice depth profiles. We demonstrate the potential of UDD by studying a thin Si single crystal upon single pulse femtosecond optical excitation. Our study reveals that below the melting threshold strong lattice distortions not only longitudinal, but also transversal to the propagation of the strain wave appear on picosecond time scales along the single crystal. The observation of this transversal deformation after laser excitation contradicts previous work that were not able to observed it, what could be related to the high sensitivity of dynamical diffraction with respect to the lattice distortions. The speed of propagation of this ultrafast transversal strain deformation is observed to be slower to the longitudinal sound speed for Si as described in the bibliography.

We investigate the ultrafast dynamics of plasma formation by optical breakdown, filamentation, and cavitation in water, using high spatiotemporal resolution offered by x-ray free-electron laser (XFEL) radiation. A femtosecond infrared laser pulse is focused in a water-filled cuvette and probed by a single femtosecond x-ray pulse, with a time delay covering nearly four orders of magnitude. By exploiting the quantitative contrast values obtained by phase retrieval, we can follow the transition from plasma to gas in terms of a continuous decrease of mass density in the cavity. At the same time, we image the emission of a cylindrical shock wave for the scenario of a single elongated breakdown filament with a high degree of symmetry. Contrarily, the regime of multiple breakdown spots deviates from cylindrical symmetry and the idealized picture expected for a Gaussian beam. Here different scenarios of cavitation and (collective) expansion dynamics as well as bubble fusion are observed. Specifically, we quantify the decrease of the expansion velocity with the number of auxiliary cavitation events due to a redistribution of the deposited laser energy. We also report events with (multi)filamentation reflecting instabilities in the initial distribution of the laser intensity upon formation of the plasma. Filaments with submicron diameter and few-micrometer spacing are observed, as well as the phenomena of filament emergence, splitting, and termination. The different regimes of heterogeneous optical breakdown and cavitation can be distinguished depending on the laser pulse energy. Altogether, the experiments demonstrate the potential of single-pulse XFEL imaging for the investigation of optical breakdown and ultrafast hydrodynamics. The future application of the imaging approach to soft matter environments, tissue, glasses, and opaque materials seems straightforward.

Understanding protein motion within the cell is crucial for predicting reaction rates and macromolecular transport in the cytoplasm. A key question is how crowded environments affect protein dynamics through hydrodynamic and direct interactions at molecular length scales. Using megahertz X-ray Photon Correlation Spectroscopy (MHz-XPCS) at the European X-ray Free Electron Laser (EuXFEL), we investigate ferritin diffusion at microsecond time scales. Our results reveal anomalous diffusion, indicated by the non-exponential decay of the intensity autocorrelation function g 2 ( q , t ) at high concentrations. This behavior is consistent with the presence of cage-trapping between the short- and long-time protein diffusion regimes. Modeling with the δ γ -theory of hydrodynamically interacting colloidal spheres successfully reproduces the experimental data by including a scaling factor linked to the protein direct interactions. These findings offer insights into the complex molecular motion in crowded protein solutions, with potential applications for optimizing ferritin-based drug delivery, where protein diffusion is the rate-limiting step.

We report on the coherence properties and characteristics of the split-and-delay unit at the Materials Imaging and Dynamics instrument of the European XFEL under seeded-beam conditions. Our investigation focuses on the speckle contrast extracted from the scattering patterns from static scatterers and pulse splitting characteristics. Seeded-beam operation enabled a high throughput of the split-and-delay unit. We highlight the invaluable potential of the split-and-delay unit for experimental investigations for enhancing our understanding of ultrafast phenomena in molecular liquids, such as water and aqueous solutions.

Phase transitions are governed by both intrinsic and extrinsic heterogeneities, yet capturing their spatio-temporal dynamics remains a challenge. While ultrafast techniques track phase changes on femtosecond timescales, the spatial complexity and stochastic nature of the processes often remain hidden. Here, we present an experimental approach that combines well-established ultrafast hard-X-ray diffraction with a propagating strain pulse as a universal and non-invasive probe. This ultrafast X-ray sonography can capture the spatio-temporal phase heterogeneity in great detail by resolving the phase-specific strain response. We apply this approach to the antiferromagnetic-to-ferromagnetic magneto-structural phase transition in FeRh and identify the ferromagnetic phase to nucleate at the surface as narrow columnar domains of approximately 30 nm diameter. Besides reconciling the diverse experimental results in the literature on FeRh, X-ray sonography offers a versatile platform for investigating a wide range of phase transitions accompanied by structural changes.

Understanding and ultimately controlling the transformations and properties of nanoscale systems, from proteins to synthetic nanomaterial assemblies, is limited by the inability to uncover their dynamics on their characteristic length and time scales. Here, we nevertheless demonstrate this ability using MHz X-ray photon correlation spectroscopy (XPCS) – directly elucidating the characteristic microsecond-dynamics of density fluctuations of semiconductor nanocrystals (NCs), not only in a colloidal dispersion but also in a liquid phase consisting of densely packed, yet mobile, NCs with no long-range order. We find the wavevector-dependent fluctuation rates in the liquid phase are suppressed relative to those in the colloidal phase and relative to observations of densely packed repulsive particles. We show that the suppressed rates are due to a substantial decrease in the self-diffusion of NCs, which we attribute to explicit attractive interactions. Using coarse-grained simulations, we find that the extracted shape and strength of the interparticle potential explains the stability of the liquid phase, in contrast to the gelation observed via XPCS in many other charged colloidal systems. This work opens the door to elucidating fast, condensed phase dynamics in complex fluids and other nanoscale soft matter, such as densely packed proteins and non-equilibrium self-assembly processes, in addition to designing microscopic strategies to avert gelation.

This article provides examples of setups and upgrades currently under development at the Materials Imaging and Dynamics (MID) instrument of the European X-Ray Free-Electron Laser (EuXFEL): the first installations of the Multi-environmental multi-Detector Setup (MDS_2), its next design scenarios in the MID Instrument and the Multi-Purpose Chamber 2 project design status, with the first successful commissioning of its Breadboard Assembly.

Single bubble sonoluminescence (SBSL) is the phenomenon of synchronous light emission due to the violent collapse of a single spherical bubble in a liquid, driven by an ultrasonic field. During the bubble collapse, matter inside the bubble reaches extreme conditions of several gigapascals and temperatures on the order of 10000 K, leading to picosecond flashes of visible light. To this day, details regarding the energy focusing mechanism rely on simulations due to the fast dynamics of the bubble collapse and spatial scales below the optical resolution limit. In this work we present phase-contrast holographic imaging with single x-ray free-electron laser (XFEL) pulses of a SBSL cavitation bubble in water. X-rays probe the electron density structure and by that provide a uniquely new view on the bubble interior and its collapse dynamics. The involved fast time-scales are accessed by sub-100 fs XFEL pulses and a custom synchronization scheme for the bubble oscillator. We find that during the whole oscillation cycle the bubble's density profile can be well described by a simple step-like structure, with the radius R following the dynamics of the Gilmore model. The quantitatively measured internal density and width of the boundary layer exhibit a large variance. Smallest reconstructed bubble sizes reach down to R similar or equal to 0.8 mu m , and are consistent with spherical symmetry. While we here achieved a spatial resolution of a few 100 nm, the visibility of the bubble and its internal structure is limited by the total x-ray phase shift which can be scaled with experimental parameters.

In this work, we study the jetting dynamics of individual cavitation bubbles using x-ray holographic imaging and high-speed optical shadowgraphy. The bubbles are induced by a focused infrared laser pulse in water near the surface of a flat, circular glass plate, and later probed with ultrashort x-ray pulses produced by an x-ray free-electron laser (XFEL). The holographic imaging can reveal essential information of the bubble interior that would otherwise not be accessible in the optical regime due to obscuration or diffraction. The influence of asymmetric boundary conditions on the jet’s characteristics is analysed for cases where the axial symmetry is perturbed and curved liquid filaments can form inside the cavity. The x-ray images demonstrate that when oblique jets impact the rigid boundary, they produce a non-axisymmetric splash which grows from a moving stagnation point. Additionally, the images reveal the formation of complex gas/liquid structures inside the jetting bubbles that are invisible to standard optical microscopy. The experimental results are analysed with the assistance of full three-dimensional numerical simulations of the Navier–Stokes equations in their compressible formulation, which allow a deeper understanding of the distinctive features observed in the x-ray holographic images. In particular, the effects of varying the dimensionless stand-off distances measured from the initial bubble location to the surface of the solid plate and also to its nearest edge are addressed using both experiments and simulations. A relation between the jet tilting angle and the dimensionless bubble position asymmetry is derived. The present study provides new insights into bubble jetting and demonstrates the potential of x-ray holography for future investigations in this field.

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.

The European X-ray Free Electron Laser (European XFEL) is a cutting-edge user facility that generates per second up to 27,000 ultra-short, spatially coherent X-ray pulses within an energy range of 0.26 to more than 20 keV. Specialized instrumentation, including various 2D X-ray detectors capable of handling the unique time structure of the beam, is required. The one-megapixel AGIPD (AGIPD1M) detectors, developed for the European XFEL by the AGIPD Consortium, are the primary detectors used for user experiments at the SPB/SFX and MID instruments. The first AGIPD1M detector was installed at SPB/SFX when the facility began operation in 2017, and the second one was installed at MID in November 2018. The AGIPD detector systems require a dedicated infrastructure, well-defined safety systems, and high-level control procedures to ensure stable and safe operation. As of now, the AGIPD1M detectors installed at the SPB/SFX and MID experimental end stations are fully integrated into the European XFEL environment, including mechanical integration, vacuum, power, control, data acquisition, and data processing systems. Specific high-level procedures allow facilitated detector control, and dedicated interlock systems based on Programmable Logic Controllers ensure detector safety in case of power, vacuum, or cooling failure. The first 6 years of operation have clearly demonstrated that the AGIPD1M detectors provide high-quality scientific results. The collected data, along with additional dedicated studies, have also enabled the identification and quantification of issues related to detector performance, ensuring stable operation. Characterization and calibration of detectors are among the most critical and challenging aspects of operation due to their complex nature. A methodology has been developed to enable detector characterization and data correction, both in near real-time (online) and offline mode. The calibration process optimizes detector performance and ensures the highest quality of experimental results. Overall, the experience gained from integrating and operating the AGIPD detectors at the European XFEL, along with the developed methodology for detector characterization and calibration, provides valuable insights for the development of next-generation detectors for Free Electron Laser X-ray sources.