English

Crystal structure optimisation using an auxiliary equation of state

Materials Science 2016-01-26 v2

Abstract

Standard procedures for local crystal-structure optimisation involve numerous energy and force calculations. It is common to calculate an energy-volume curve, fitting an equation of state around the equilibrium cell volume. This is a computationally intensive process, in particular for low-symmetry crystal structures where each isochoric optimisation involves energy minimisation over many degrees of freedom. Such procedures can be prohibitive for non-local exchange-correlation functionals or other 'beyond' density functional theory electronic structure techniques, particularly where analytical gradients are not available. We present a simple approach for efficient optimisation of crystal structures based on a known equation of state. The equilibrium volume can be predicted from one single-point calculation, and refined with successive calculations if required. The approach is validated for PbS, PbTe, ZnS and ZnTe using nine density functionals, and applied to the quaternary semiconductor Cu2_{2}ZnSnS4_{4} and the magnetic metal-organic framework HKUST-1.

Keywords

Cite

@article{arxiv.1507.08815,
  title  = {Crystal structure optimisation using an auxiliary equation of state},
  author = {Adam J. Jackson and Jonathan M. Skelton and Christopher H. Hendon and Keith T. Butler and Aron Walsh},
  journal= {arXiv preprint arXiv:1507.08815},
  year   = {2016}
}
R2 v1 2026-06-22T10:23:15.180Z