Quantum lattice dynamics and their importance in ternary superhydride clathrates

Abstract

Abstract The quantum nature of the hydrogen lattice in superconducting hydrides can have crucial effects on the material’s properties. Taking a detailed look at the dynamic stability of the recently predicted BaSiH8 phase, we find that the inclusion of anharmonic quantum ionic effects leads to an increase in the critical dynamical pressure to 20 GPa as compared to 5 GPa within the harmonic approximation. We identify the change in the crystal structure due to quantum ionic effects to be the main driving force for this increase and demonstrate that this can already be understood at the harmonic level by considering zero-point energy corrections to the total electronic energy. In fact, the previously determined critical pressure of kinetic stability p kin = 30 GPa still poses a stricter bound for the synthesizability of BaSiH8 and similar hydride materials than the dynamical stability and therefore constitutes a more rigorous and accurate estimate for the experimental realizability of these structures.