Determination of ground-state and low-energy structures of perovskite superlattices from first principles

Abstract

In the development of first-principles high-throughput searches for materials with desirable functional properties, there is a clear need for an efficient method to determine the ground state and low-energy alternative structures of superlattices. A method based on a simple strategy -- to generate starting structures based on low-energy structures of the constituent compounds, which are then optimized via structural relaxation calculations -- is proposed. This "stacking method" is demonstrated on the 2:2 PbTiO$_3$/SrTiO$_3$ superlattice, which has been the subject of recent experimental and theoretical interest. Considerations relevant to wider use of the method are discussed.