Stability of calcium and magnesium carbonates at lower mantle thermodynamic conditions

Quaternary CaO-MgO-Al2O3-SiO2 glasses are important constituents of the Earth's lower crust and mantle, and they also have important industrial applications such as in metallurgical processes, concrete production and emerging low-CO2 cement technologies. In particular, these applications rely heavily on the composition-structure-reactivity relationships for CMAS glasses, which are not yet well established. In this study, we developed a robust method that combines force-field ...

Bridgmanite, a high temperature and pressure form of $MgSiO_3$, is believed to be Earth's most abundant mineral and responsible for the observed seismic anisotropy in the mantle. Little is known about surfaces of bridgmanite but knowledge of the most stable surface terminations is important for understanding various geochemical processes as well as likely slip planes. A density functional theory based thermodynamic approach is used here to establish the range of stability of ...

There is a direct relation between the composition of a host star and that of the planets orbiting around it. As such, the recent discovery of stars with unusual chemical composition, notably enriched in carbon instead of oxygen, support the existence of exoplanets with a chemistry dominated by carbides instead of oxides. Accordingly several studies have been recently conducted on the Si C binary system at high pressure and temperature. Nonetheless, the properties of carbides...

(Mg, Fe)SiO$_3$ post-perovskite is the highest pressure silicate mineral phase in the Earth's interior. The extreme pressure and temperature conditions inside large extrasolar planets will likely lead to phase transitions beyond pPv. In this work we have explored the high-pressure phase relations in Mg$_2$SiO$_4$ using computations based on density functional theory. We find that a partially disordered I-42d type structure would be stable in the interiors of these super-Earth...

Reports on the detection of carbonates in planetary nebulae (PNe) and protostars suggested the existence of a mechanism that produce these compounds in stellar winds and outflows. A consecutive laboratory study reported a possible mechanism by observing the non-thermodynamic equilibrium (TE), gas-phase condensation of amorphous silicate grains with amorphous calcium carbonate inclusions. It concluded that water vapor was necessary to the formation of the carbonates. We presen...

The stability of possible termination structures for the (010) surface of forsterite, $ Mg_2SiO_4 $, is studied using a density functional theory (DFT) based thermodynamic approach. The DFT calculations are used to estimate the surface Gibbs free energy of various surface structures and compare their stability as a function of the chemical environment. Among 9 possible terminations, the SiO-II, M2, O-II terminations are found to be most stable as conditions range from Mg-poor...

Lattice thermal conductivity ($\kappa_{lat}$) of MgSiO$_3$ postperovskite (MgPPv) under the Earth's lower mantle high pressure-temperature conditions is studied using the phonon quasiparticle approach by combing \textit{ab initio} molecular dynamics and lattice dynamics simulations. Phonon lifetimes are extracted from the phonon quasiparticle calculations, and the phonon group velocities are computed from the anharmonic phonon dispersions, which in principle capture full anha...

Calcium carbonate plays a crucial role in the global carbon cycle, and its phase diagram has always been of significant scientific interest. In this study, we used molecular dynamics (MD) to investigate several structural phase transitions of calcium carbonate. Using the Raiteri potential model, we explored the structural transitions occurring at a constant pressure of 1 bar with temperatures ranging from 300 K to 2500 K, and at a constant temperature of 1600 K with pressures...

We present a new technique which allows the fully {\em ab initio} calculation of the chemical potential of a substitutional impurity in a high-temperature crystal, including harmonic and anharmonic lattice vibrations. The technique uses the combination of thermodynamic integration and reference models developed recently for the {\em ab initio} calculation of the free energy of liquids and anharmonic solids. We apply the technique to the case of the substitutional oxygen impur...

As the number of detected rocky extrasolar planets increases, the question of whether their surfaces could be habitable is becoming more pertinent. On Earth, the long-term carbonate silicate cycle is able to regulate surface temperatures over timescales larger than one million years. Elevated temperatures enhance weathering, removing CO$_2$ from the atmosphere, which is subducted into the mantle. At mid-ocean ridges, CO$_2$ is supplied to the atmosphere from the interior. The...