Virp: neural network-accelerated prediction of physical properties in site-disordered materials

Abstract

Among metallic alloys, ceramics, and even common compounds such as water ice, it is usual to find materials in which crystalline order is expressed as a probability. In such cases, one or more sites within a crystal can be occupied by multiple elements or vacancies, according to a set of probabilities. These crystal structures remain inaccessible to common first-principles materials simulation methodologies, which assumes perfect crystal order. Workaround strategies to this limitation include quasirandom structures and cluster expansion. These methods are system-specific and computationally expensive as they rely on large scale Monte Carlo simulations of enlarged unit cells. To address these limitations, we propose a pipeline combining a permutation-based virtual cell generation algorithm, sampling regime, and thermodynamic post-processing which greatly improves the feasibility of computation analyses for site-disordered materials. We demonstrate that the massive configurational space can be adequately sampled with 400 virtual cells, as long as the supercell definition is sufficiently large.