Simulation of Material Properties Below the Debye Temperature: A Path-Integral Molecular Dynamics Case Study of Quartz

Abstract

Classical and path integral molecular dynamics (PIMD) simulations are used to study alpha-quartz and beta-quartz in a large range of temperatures at zero external stress. PIMD account for quantum fluctuations of atomic vibrations, which can modify material properties at temperatures below the Debye temperature. The difference between classical and quantum mechanical results for bond lengths, bond angles, elastic modulii, and some dynamical properties is calculated and comparison to experimental data is done. Only quantum mechanical simulations are able to reflect the correct thermomechanical properties below room temperature. It is discussed in how far classical and PIMD simulations can be helpful in constructing improved potential energy surfaces for silica.