Equations of state and phase transitions in (Mg,Fe)SiO3 perovskite and post-perovskites, position of the phase boundary and its double crossing, by Quantum Monte Carlo

Abstract:

We have performed quantum Monte Carlo (QMC) simulations and density functional theory calculations to study the equations of state and phase transitions in (Mg,Fe)SiO3 perovskite (Pv, bridgmanite) and post-perovskite (PPv) .[1] The ground-state energies were derived using quantum QMC simulations and the temperature-dependent Helmholtz free energies were calculated within the quasiharmonic approximation and density functional perturbation theory. Quantum Monte Carlo (QMC) within Diffusion Monte Carlo (DMC) is a stochastic numerical solution of Schrödinger’s equation within the fixed many-particle nodes obtained, in our case, from a determinant of DFT orbitals. Agreement with experiments is improved over DFT alone. Furthermore, we obtain statistical error bounds on the results, rather than the unconstrained errors of DFT. The Pv-PPv phase boundary calculated from our QMC equations of state is also consistent with experiments, and better than previous DFT computations. In order to understand the H-phase reported in (Mg,Fe)SiO3 [2], we have performed evolutionary structure searching for FeSiO3.[3] We find a new structure type which may be consistent with the experimental observations, but is a lower pressure, less dense, phase. We have built a thermodynamic model for (Mg,Fe)SiO3 perovskite as a function of P and T, and will discuss implications for the location of the phase boundary in D’’ and its double crossing [4]. This work is supported by NSF and the ERC Advanced Grant ToMCaT.

[1] Y. Lin, R. E. Cohen, S. Stackhouse, K. P. Driver, B. Militzer, L. Shulenburger, and J. Kim, Phys. Rev. B 90 (2014).
[2] L. Zhang et al., Science 344, 877 (2014).
[3] R. E. Cohen and Y. Lin, Phys. Rev. B 90 (2014).
[4] J.W. Hernlund, C. Thomas and P.J. Tackley, Nature 434, 882 (2005).