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Sub-picosecond optical laser processing of metals is actively utilized for modification of a heated surface layer. But for deeper modification of different materials a laser in the hard x-ray range is required. Here, we demonstrate that a single 9-keV x-ray pulse from a free-electron laser can form a um-diameter cylindrical cavity with length of ~1 mm in LiF surrounded by shock-transformed material. The plasma-generated shock wave with TPa-level pressure results in damage, melting and polymorphic transformations of any material, including transparent and non-transparent to conventional optical lasers. Moreover, cylindrical shocks can be utilized to obtain a considerable amount of exotic high-pressure polymorphs. Pressure wave propagation in LiF, radial material flow, formation of cracks and voids are analyzed via continuum and atomistic simulations revealing a sequence of processes leading to the final structure with the long cavity. Similar results can be produced with semiconductors and ceramics, which opens a new pathway for development of laser material processing with hard x-ray pulses.

We present measurements on Fe$_2$O$_3$ amorphization and melt under laser-driven shock compression up to 209(10) GPa via time-resolved in situ x-ray diffraction. At 122(3) GPa, a diffuse signal is observed indicating the presence of a non-crystalline phase. Structure factors have been extracted up to 182(6) GPa showing the presence of two well-defined peaks. A rapid change in the intensity ratio of the two peaks is identified between 145(10) and 151(10) GPa, indicative of a phase change. Present DFT+$U$ calculations of temperatures along Fe$_2$O$_3$ Hugoniot are in agreement with SESAME 7440 and indicate relatively low temperatures, below 2000 K, up to 150 GPa. The non-crystalline diffuse scattering is thus consistent with the - as yet unreported - shock amorphization of Fe$_2$O$_3$ between 122(3) and 145(10) GPa, followed by an amorphous-to-liquid transition above 151(10) GPa. Upon release, a non-crystalline phase is observed alongside crystalline $\alpha$-Fe$_2$O$_3$. The extracted structure factor and pair distribution function of this release phase resemble those reported for Fe$_2$O$_3$ melt at ambient pressure., Comment: 11 pages, 4 figures, under review

Mosaic crystals, with their high integrated reflectivities, are widely-employed in spectrometers used to diagnose high energy density systems. X-ray Thomson scattering (XRTS) has emerged as a powerful diagnostic tool of these systems, providing in principle direct access to important properties such as the temperature via detailed balance. However, the measured XRTS spectrum is broadened by the spectrometer instrument function (IF), and without careful consideration of the IF one risks misdiagnosing system conditions. Here, we consider in detail the IF of 40 $\mu$m and 100 $\mu$m mosaic HAPG crystals, and how the broadening varies across the spectrometer in an energy range of 6.7-8.6 keV. Notably, we find a strong asymmetry in the shape of the IF towards higher energies. As an example, we consider the effect of the asymmetry in the IF on the temperature inferred via XRTS for simulated 80 eV CH plasmas, and find that the temperature can be overestimated if an approximate symmetric IF is used. We therefore expect a detailed consideration of the full IF will have an important impact on system properties inferred via XRTS in both forward modelling and model-free approaches., Comment: 19 pages, 13 figures

Particle-in-Cell (PIC) method is a powerful plasma simulation tool for investigating high-intensity femtosecond laser-matter interaction. However, its simulation capability at high-density plasmas around the Fermi temperature is considered to be inadequate due, among others, to the necessity of implementing atomic-scale collisions. Here, we performed a one-dimensional with three-velocity space (1D3V) PIC simulation that features the realistic collision frequency around the Fermi temperature and atomic-scale cell size. The results are compared with state-of-the-art experimental results as well as with hydrodynamic simulation. We found that the PIC simulation is capable of simulating the nanoscale dynamics of solid-density plasmas around the Fermi temperature up to $\sim$2~ps driven by a laser pulse at the moderate intensity of $10^{14-15}$~$\mathrm{W/cm^{2}}$, by comparing with the state-of-the-art experimental results. The reliability of the simulation can be further improved in the future by implementing multi-dimensional kinetics and radiation transport.

Femtosecond high-intensity laser pulses at intensities surpassing $10^{14} \,\text{W}/\text{cm}^2$ can generate a diverse range of functional surface nanostructures. Achieving precise control over the production of these functional structures necessitates a thorough understanding of the surface morphology dynamics with nanometer-scale spatial resolution and picosecond-scale temporal resolution. In this study, we show that individual XFEL pulses can elucidate structural changes on surfaces induced by laser-generated plasmas, employing grazing-incidence small-angle x-ray scattering (GISAXS). Using aluminum-coated multilayer samples we can differentiate between ultrafast surface morphology dynamics and subsequent subsurface density dynamics, achieving nanometer-depth sensitivity and subpicosecond temporal resolution. The observed subsurface density dynamics serve to validate advanced simulation models depicting matter under extreme conditions. Our findings promise to unveil novel avenues for laser material nanoprocessing and high-energy-density science., Comment: 11 pages, 5 figures. This is the version of the article before peer review

Optimizing grain boundary characteristics in polycrystalline materials can improve their properties. Many processing methods have been developed for grain boundary manipulation, including the use of intense radiation in certain applications. In this work, we used X-ray free electron laser pulses to irradiate single-crystalline bismuth selenide (Bi2Se3) and observed grain boundary formation and subsequent grain rotation in response to the X-ray radiation. Our observations with simultaneous transmission X-ray microscopy and X-ray diffraction demonstrate how intense X- ray radiation can rapidly change size and texture of grains., Comment: 37 pages, 11 figures including 6 supplemental figures

Using a novel ultrahigh resolution ($\Delta E \sim 0.1\,$eV) 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 ab initio 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.

The last decade has shown the great potential that X-ray Free Electron Lasers (FEL) have to study High Energy Density (HED) matter. Experiments at FELs have made significant breakthroughs in Shock Physics and Dynamic Diffraction, Dense Plasma Physics and Warm Dense Matter Science, using techniques such as isochoric heating, inelastic scattering, small angle scattering and x-ray diffraction. In addition, and complementary to these techniques, the coherent properties of the FEL beam can be used to image HED samples with high fidelity. We present new imaging diagnostics and techniques developed at the Matter in Extreme Conditions (MEC) instrument at Linac Coherent Light Source (LCLS) over the last few years. We show results in Phase Contrast Imaging geometry, where the X-ray beam propagates from the target to a camera revealing its phase, as well as in Direct Imaging geometry, where a real image of the sample plane is produced in the camera with a spatial resolution down to 200 nm. Last, we show an implementation of the Talbot Imaging method allowing both x-ray phase and intensity measurements change introduced by a target with sub-micron resolution.

At modern X-ray sources, such as synchrotrons and X-ray Free-Electron Lasers (XFELs), it is important to measure the absolute value of the photon energy directly. Here, a method for absolute spectral metrology is presented. A photon energy estimation method based on the spectral measurements and rocking of diffracting crystals is presented. The photon energy of SASE1 channel of the European XFEL was measured, and the benefits and applications of the precise photon energy evaluation are discussed.

Materials exposed to ultrashort intense x-ray irradiation may experience various damaging conditions depending on the in-situ temperature. A pre-heated target exposed to intense x-rays plays a crucial role in numerous systems of physical-technical importance, ranging from the heavily-, and repeatedly radiation-loaded optics at x-ray free-electron laser facilities, to the first wall of prospective inertial fusion reactors. We study theoretically the damage threshold dependence on the temperature in different classes of materials: an insulator (diamond), a semiconductor (silicon), a metal (tungsten), and an organic polymer (PMMA). The numerical techniques used here enable us to trace the evolution of both, an electronic state and atomic dynamics of the materials. It includes damage mechanisms such as thermal damage (induced by an increase of the atomic temperature due to energy transfer from x-ray-excited electrons) and nonthermal phase transitions (induced by changes in the interatomic potential due to excitation of electrons). We demonstrate that in the pre-heated materials, typically, the thermal damage threshold stays the same or lowers with the increase of the in-situ temperature, whereas nonthermal damage thresholds may be lowered or raised, depending on the particular material and specifics of the damage kinetics.

Observing ultrafast laser-induced structural changes in nanoscale systems is essential for understanding the dynamics of intense light-matter interactions. For laser intensities on the order of $10^{14} \, \rm W/cm^2$, highly-collisional plasmas are generated at and below the surface. Subsequent transport processes such as heat conduction, electron-ion thermalization, surface ablation and resolidification occur at picosecond and nanosecond time scales. Imaging methods, e.g. using x-ray free-electron lasers (XFEL), were hitherto unable to measure the depth-resolved subsurface dynamics of laser-solid interactions with appropriate temporal and spatial resolution. Here we demonstrate picosecond grazing-incidence small-angle x-ray scattering (GISAXS) from laser-produced plasmas using XFEL pulses. Using multi-layer (ML) samples, both the surface ablation and subsurface density dynamics are measured with nanometer depth resolution. Our experimental data challenges the state-of-the-art modeling of matter under extreme conditions and opens new perspectives for laser material processing and high-energy-density science., Comment: 16 pages, 4 figures. This is the version of the article before peer review, as submitted by authors. There is a Supplementary Information file in the Ancillary files directory

Ultrafast dynamics are generally investigated using stroboscopic pump-probe measurements, which characterize the sample properties for a single, specific time delay. These measurements are then repeated for a series of discrete time delays to reconstruct the overall time trace of the process. As a consequence, this approach is limited to the investigation of fully reversible phenomena. We recently introduced an off-axis zone plate based X-ray streaking technique, which overcomes this limitation by sampling the relaxation dynamics with a single femtosecond X-ray pulse streaked over a picosecond long time window. In this article we show that the X-ray absorption cross section can be employed as the contrast mechanism in this novel technique. We show that changes of the absorption cross section on the percent level can be resolved with this method. To this end we measure the ultrafast magnetization dynamics in CoDy alloy films. Investigating different chemical compositions and infrared pump fluences, we demonstrate the routine applicability of this technique. Probing in transmission the average magnetization dynamics of the entire film, our experimental findings indicate that the demagnetization time is independent of the specific infrared laser pump fluence. These results pave the way for the investigation of irreversible phenomena in a wide variety of scientific areas., Comment: 9 pages, 5 figures

The demands on optical components to tolerate high radiation dose and manipulate hard x-ray beams that can fit the experiment requirements, are constantly increasing due to the advancements in the available x-ray sources. Here we have successfully fabricated the transmission type gratings using diamond, with structure sizes ranging from few tens of nanometres up to micrometres, and aspect ratio of up to 20. The efficiencies of the gratings were measured over a wide range of photon energies and their radiation tolerance was confirmed using the most intense x-ray source in the world. The fidelity of these grating structures was confirmed by the quality of the measured experimental results.