Abstract Oxygen and other light elements comprise up to 5 wt% of the Earth’s outer-core, and may significantly influence its physical properties and the operation of the geodynamo. Here we report in situ X-ray diffraction measurements of Fe, Fe + 4.5 FeO (atomic proportion), and Fe 2 O 3 melts at 177-440 GPa, achieved using laser-driven shock compression at an x-ray free-electron laser. The melts exhibit Fe-O coordination numbers between 4.0(0.4) and 4.5(0.4), indicating predominantly four-fold coordination environments. These coordination states are significantly smaller than those of Fe-bearing lower-mantle phases such as bridgmanite and ferropericlase. Shorter Fe-Fe interatomic distances in compressed iron oxide melts drive the denser packing relative to ambient melts, while the structural differences between Fe + 4.5 FeO and Fe 2 O 3 melts under shock indicate that the oxidation state modulates oxygen solubility in liquid Fe. At 177 GPa ( ~ 380 km below the core-mantle boundary) and 3800 K, Fe 2 O 3 melts exhibit higher Fe-O coordination, suggesting that local variations in oxygen content could contribute to the stratification in the uppermost outer-core inferred from seismological and geomagnetic observations.

Flyer impact experiments are performed through different techniques (gas gun, electrical drivers, laser). Each technique presents advantages but also some limitations such as flyer integrity, flatness or dimensions uncertainty. To overcome these issues, we proposed a new technique using laser direct irradiation and based on LASAT principle.\\ Aluminium flyers are accelerated from 0.5 to 4.3 km/s. Velocity measurements are performed with different diagnostics (line-VISAR, PDV, shadowgraphy). A predictive model for flyer velocity depending on laser intensity, and using Rankine-Hugoniot equations, is presented and is in good agreement with experimental measurement. Flyer flatness and debris ejection are investigated as well as flyer curve shapping is mentioned. Two hypervelocity impacts (3.2 - 3.8 km/s) are performed on porous graphite as exploratory work. Comparison with simulation results suggests that the current flyer technique may be used for impact studies.

The robust diagnosis of conditions generated in warm dense matter experiments remains a persistent challenge. Here, we describe the measurement of shock-compressed aluminium at 50 GPa with angle-resolved femtosecond x-ray Thomson scattering (XRTS) over a wide range of scattering wave vectors at the European X-Ray Free-Electron Laser. The measured plasmon dispersion and line shape show that the de facto standard approach for analyzing XRTS spectra, using uniform-electron-gas models, systematically overestimates the resonance energy by up to 8 eV. We present an approach using ab initio methods that agrees within the experimental uncertainty and demonstrates how accounting for shock-induced disorder in shock-compressed systems is critical for their understanding, providing evidence that ab initio treatments are required for reliable XRTS inference in warm dense aluminium.

Oxygen and other light elements comprise up to 5 wt

We present 50-fs, single-shot measurements of the x-ray thermal diffuse scattering (TDS) from copper foils that have been shocked via nanosecond laser ablation up to pressures above ∼135 GPa. We hence deduce the x-ray Debye–Waller factor, providing a temperature measurement. The targets were laser-shocked with the DiPOLE 100-X laser at the High Energy Density endstation of the European X-ray Free-Electron Laser. Single x-ray pulses, with a photon energy of 18 keV, were scattered from the samples and recorded on Varex detectors. Despite the targets being highly textured (as evinced by large variations in the elastic scattering) and with such texture changing upon compression, the absolute intensity of the azimuthally averaged inelastic TDS between the Bragg peaks is largely insensitive to these changes, and allowing for both Compton scattering and the low-level scattering from a sacrificial ablator layer provides a reliable measurement of T/ΘD2, where ΘD is the Debye temperature. We compare our results with the predictions of the SESAME 3336 and LEOS 290 equations of state for copper and find good agreement within experimental errors. We, thus, demonstrate that single-shot temperature measurements of dynamically compressed materials can be made via thermal diffuse scattering of XFEL radiation.

Carbonate minerals are important in Earth's system sciences and have been found on Mars and in meteorites and asteroids, highlighting the importance of impacts in planetary processes. While extensively studied under static compression, the behavior of carbonates under shock compression remains underexplored, with no in situ X-ray investigations reported so far. Here we investigate natural magnesiosiderite (Fe_0.6Mg_0.4CO_3) under nanosecond laser-driven shock compression at pressures up to 150 GPa, coupled with in situ ultrafast synchrotron X-ray absorption spectroscopy (XAS). The interpretation of the experimental spectra is complemented using first-principles absorption cross-section calculations performed on crystalline phases at different pressures and on a dense liquid phase obtained using density functional theory-based molecular dynamics (DFT-MD) simulations. Under laser-driven shock compression, the magnesiosiderite crystal phase remains unchanged up to the melt. Under shock reverberation, the absorption spectra show changes similar to those attributed to a high-spin to low-spin transition observed under static compression. At higher pressures, the laser shock induces the formation of CO_4 tetrahedral units in the melt. Upon unloading from the shocked state, only a few nanoseconds later, the original magnesiosiderite phase is recovered.

We present measurements on Fe2O3 amorphization and melt under laser-driven shock compression up to 209(10) GPa via time-resolved x-ray diffraction. At 122(3) GPa, a diffuse signal is observed indicating the presence of a noncrystalline 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(12) and 151(12) GPa, indicative of a phase change. The noncrystalline diffuse scattering is consistent with shock amorphization of Fe2O3 between 122(3) and 145(12) GPa, followed by an amorphous-to-liquid transition above 151(12) GPa. Upon release, a noncrystalline phase is observed alongside crystalline α−Fe2O3. The extracted structure factor and pair distribution function of this release phase resemble those reported for Fe2O3 melt at ambient pressure. Published by the American Physical Society 2025

X-ray free electron laser (XFEL) sources coupled to high-power laser systems offer an avenue to study the structural dynamics of materials at extreme pressures and temperatures. The recent commissioning of the DiPOLE 100-X laser on the high energy density (HED) instrument at the European XFEL represents the state-of-the-art in combining x-ray diffraction with laser compression, allowing for compressed materials to be probed in unprecedented detail. Here, we report quantitative structural measurements of molten Sn compressed to 85(5) GPa and ∼3500 K. The capabilities of the HED instrument enable liquid density measurements with an uncertainty of ∼1% at conditions which are extremely challenging to reach via static compression methods. We discuss best practices for conducting liquid diffraction dynamic compression experiments and the necessary intensity corrections which allow for accurate quantitative analysis. We also provide a polyimide ablation pressure vs input laser energy for the DiPOLE 100-X drive laser which will serve future users of the HED instrument.

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.

We report here an equation-of-state measurement of Fe2O3 obtained with laser-driven shock compression. The data are in excellent agreement with previous dynamic and static compression measurements at low pressure, and extend the known Hugoniot up to 700 GPa. We observe a large volume drop of '10% at 86 GPa, which could be associated, according to static compression observations, with the iron spin transition. Our measurements also suggest a change of the Hugoniot curve between 150 and 250 GPa. Above 250 GPa and within our error bars, we do not observe significant modifications up to the maximum pressure of 700 GPa reached in our experiment.

Resonant inelastic x-ray scattering (RIXS) is a widely used spectroscopic technique, providing access to the electronic structure and dynamics of atoms, molecules, and solids. However, RIXS requires a narrow bandwidth x-ray probe to achieve high spectral resolution. The challenges in delivering an energetic monochromated beam from an x-ray free electron laser (XFEL) thus limit its use in few-shot experiments, including for the study of high energy density systems. Here we demonstrate that by correlating the measurements of the self-amplified spontaneous emission (SASE) spectrum of an XFEL with the RIXS signal, using a dynamic kernel deconvolution with a neural surrogate, we can achieve electronic structure resolutions substantially higher than those normally afforded by the bandwidth of the incoming x-ray beam. We further show how this technique allows us to discriminate between the valence structures of Fe and Fe$_2$O$_3$, and provides access to temperature measurements as well as M-shell binding energies estimates in warm-dense Fe compounds.

We present in-situ x-ray diffraction and velocity measurements of Fe$_2$O$_3$ under laser shock compression at pressures between 38-116 GPa. None of the phases reported by static compression studies were observed. Instead, we observed an isostructural phase transition from $\alpha$-Fe$_2$O$_3$ to a new $\alpha^\prime$-Fe$_2$O$_3$ phase at a pressure of 50-62 GPa. The $\alpha^\prime$-Fe$_2$O$_3$ phase differs from $\alpha$-Fe$_2$O$_3$ by an 11% volume drop and a different unit cell compressibility. We further observed a two-wave structure in the velocity profile, which can be related to an intermediate regime where both $\alpha$ and $\alpha^\prime$ phases coexist. Density functional theory calculations with a Hubbard parameter indicate that the observed unit cell volume drop can be associated with a spin transition following a magnetic collapse.

The insulator–metal transition in liquid hydrogen is an important phenomenon to understand the interiors of gas giants, such as Jupiter and Saturn, as well as the physical and chemical behavior of materials at high pressures and temperatures. Here, the path toward an experimental approach is detailed based on spectrally resolved x-ray scattering, tailored to observe and characterize hydrogen metallization in dynamically compressed hydrocarbons in the regime of carbon–hydrogen phase separation. With the help of time-dependent density functional theory calculations and scattering spectra from undriven carbon samples collected at the European x-ray Free-Electron Laser Facility (EuXFEL), we demonstrate sufficient data quality for observing C–H demixing and investigating the presence of liquid metallic hydrogen in future experiments using the reprated drive laser systems at EuXFEL.

We report on ion emission from plasma produced on thick targets irradiated with nanosecond and femtosecond pulses delivered by mid-ultraviolet and soft x-ray lasers, respectively. To distinguish between different ion acceleration mechanisms, the maximum kinetic energy of ions produced under different interaction conditions is plotted versus laser fluence. The transformation of the time-of-flight detector signal into ion charge density distance-of-flight spectra makes it possible to determine the mean kinetic energy of the fastest ion groups based on the influence of the acoustic velocity of ion expansion. This allows obtaining additional characteristics of the ion production. The final energy of the group of fast ions determined using the ion sound velocity model is an order of magnitude larger in the fs-XFEL interaction than in the ns-UV one. On the contrary, the ablation yield of ions in our experiment is seven orders of magnitude greater when applying ns-UV laser pulses, not only due to higher energies of UV laser pulses, but also due to a significant difference in interaction and ion formation mechanisms.

In this study, we investigated phase transformations of CaTiO3 perovskite using x-ray diffraction at high pressure and high temperature up to 170 GPa and 4500 K in a laser-heated diamond-anvil cell. We report a high-pressure dissociation of CaTiO3 into CaO-B2 and CaTi2O5 with a monoclinic P2/m structure, instead of the expected transformation of the orthorhombic distorted perovskite structure into a post-perovskite phase. We propose that this transition may be favored by the B1 to B2 phase change of CaO at around 60 GPa. In order to provide additional information on the high pressure properties of CaTiO3 perovskite, we measured its melting temper-ature using CO2 laser heated diamond anvil cell up to 55 GPa yielding a fit of the melting curve to a Kraut-Kennedy empirical law according to: Tm (K) = 2188 * [1 + 4.23 * (Delta V/V0)]. To provide some further insight into the thermodynamic properties of CaTiO3, we determined the P-V-T equation of state of the orthorhombic mineral perovskite, fitted by using a third order Birch-Murnaghan equation of state and a Berman thermal expansion model. The fit of the data yields to K0 = 180.6(4) GPa, K ' 0 = 4 (fixed), partial differential K/ partial differential T =-0.022(1) GPa K-1, alpha 1 = 3.25(5) x 10-5 K-1, alpha 2 = 1.3(1) x 10-8 K-2

X-ray Absorption Spectroscopy (XAS) is a widely used X-ray diagnostic method for studying electronic and structural properties of matter. At first glance, the relatively narrow bandwidth and the highly fluctuating spectral structure of X-ray Free Electron Lasers (XFEL) sources seem to require accumulation over many shots to achieve high data quality. To date the best approach to implementing XAS at XFEL facilities has been using monochromators to scan the photon energy across the desired spectral range. While this is possible for easily reproducible samples such as liquids, it is incompatible with many important systems. Here, we demonstrate collection of single-shot XAS spectra over 10s of eV using an XFEL source, with error bars of only a few percent. We additionally show how to extend this technique over wider spectral ranges towards Extended X-ray Absorption Fine Structure measurements, by concatenating a few tens of single-shot measurements. Our results pave the way for future XAS studies at XFELs, in particular those in the femtosecond regime. This advance is envisioned to be especially important for many transient processes that can only be initiated at lower repetition rates, for difficult to reproduce excitation conditions, or for rare samples, such as those encountered in high-energy density physics.

Results of the 2018 commissioning and experimental campaigns of the new High Power Laser Facility on the Energy-dispersive X-ray Absorption Spectroscopy (ED-XAS) beamline ID24 at the ESRF are presented. The front-end of the future laser, delivering 15 J in 10 ns, was interfaced to the beamline. Laser-driven dynamic compression experiments were performed on iron oxides, iron alloys and bismuth probed by online time-resolved XAS.

The x-ray free electron laser (XFEL) enables probing a highly compressed material response at the subnanosecond timescale. We exploit the ultrafast XFEL pulse to combine reflection x-ray diffraction and laser-driven shock compression to perform a study of the phase transformation and stability in Fe and Fe-Si alloys. Our approach enables us to observe that solid-solid phase transformations occur in Fe and Fe-Si-8.5 wt % in <= 130 ps at similar to 130 GPa; no transformation is observed in Fe-Si-16 wt % up to 110 GPa. Density functional theory calculations predict similar phase relations.