$\textit{In situ}$ time-resolved X-ray absorption spectroscopy of shock-loaded magnesiosiderite

Abstract

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 $\textit{in situ}$ X-ray investigations reported so far. Here we investigate natural magnesiosiderite (Fe$_{0.6}$Mg$_{0.4}$CO$_{3}$) under nanosecond laser-driven shock compression at pressures up to 150 GPa, coupled with $\textit{in situ}$ 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.