Dr Celine Crepisson

Abstract:

Abstract:

Experimental benchmarking of transport coefficients under extreme conditions is required for validation of differing theoretical models. To date, measurement of transport properties of dynamically compressed samples remains a challenge with only a limited number of studies able to quantify transport in high pressure and temperature matter. X-ray photon correlation spectroscopy utilizes coherent X-ray sources to measure time correlations of density fluctuations, thus providing measurements of length and time scale dependent transport properties. Here,we present a first-of-a-kind experiment to conduct X-ray photon correlation spectroscopy in laser shock compression experiments. We report measurement of the turbulent velocity in the wake of a laser driven supersonic shock and place an upper bound on thermal diffusivity in a solid density plasma on nanosecond timescales.

Abstract:

High-quality total scattering data, a key tool for understanding atomic-scale structure in disordered materials, require stable instrumentation and access to high momentum transfers. This is now routine at dedicated synchrotron instrumentation using high-energy X-ray beams, but it is very challenging to measure a total scattering dataset in less than a few microseconds. This limits their effectiveness for capturing structural changes that occur at the much faster timescales of atomic motion. Current X-ray free-electron lasers (XFELs) provide femtosecond-pulsed X-ray beams with maximum energies of ~24 keV, giving the potential to measure total scattering and the attendant pair distribution functions (PDFs) on femtosecond timescales. Here, we show that this potential has been realised using the HED scientific instrument at the European XFEL and present normalised total scattering data for 0.35Å−1 < Q < 16.6Å−1 and their PDFs from a broad spectrum of materials, including crystalline, nanocrystalline and amorphous solids, liquids, and clusters in solution. We analyse the data using a variety of methods, including Rietveld refinement, small-box PDF refinement, joint reciprocal–real space refinement, cluster refinement, and Debye scattering analysis. The resolution function of the setup is also characterised. We conclusively show that high-quality data can be obtained from a single ~30 fs XFEL pulse for multiple different sample types. Our efforts not only significantly increase the existing maximum reported Q-range for an S(Q) measured at an XFEL but also mean that XFELs are now a viable X-ray source for the broad community of people using reciprocal space total scattering and PDF methods in their research.

Abstract:

We present in situ x-ray diffraction and velocity measurements of Fe2⁢O3 under laser shock compression at pressures between 38–122 GPa. None of the high-pressure phases reported by static compression studies were observed. Instead, we observed an isostructural phase transition from 𝛼−Fe2⁢O3 to a new 𝛼′−Fe2⁢O3 phase at a pressure of 50–62 GPa. The 𝛼′−Fe2⁢O3 phase differs from 𝛼−Fe2⁢O3 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 𝛼 and 𝛼′ 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.

Abstract:

We present measurements on Fe₂O₃ 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 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.