Dynamic stabilization of cubic CaSi O3 perovskite at high temperatures and pressures from ab initio molecular dynamics

The stability of cubic CaSiO3 perovskite (CaPv) at high temperatures and pressures is investigated by vibrational normal-mode analysis. We compute power spectra of mode autocorrelation functions using a recently developed hybrid approach combining ab initio molecular dynamics with lattice dynamics. These power spectra, together with the probability distributions of atomic displacements, indicate that cubic CaPv is stabilized at T∼600 K and P∼ 26 GPa. We then utilize the concept of phonon quasiparticles to characterize the vibrational properties of cubic CaPv at high temperature and obtain anharmonic phonon dispersions through the whole Brillouin zone. Such temperature-dependent phonon dispersions pave the way for more accurate calculations of free-energy, thermodynamic, and thermoelastic properties of cubic CaPv at Earth's lower mantle conditions.