A posteriori error estimator for adaptive local basis functions to solve Kohn-Sham density functional theory

Abstract

Kohn-Sham density functional theory is one of the most widely used electronic structure theories. The recently developed adaptive local basis functions form an accurate and systematically improvable basis set for solving Kohn-Sham density functional theory using discontinuous Galerkin methods, requiring a small number of basis functions per atom. In this paper we develop residual-based a posteriori error estimates for the adaptive local basis approach, which can be used to guide non-uniform basis refinement for highly inhomogeneous systems such as surfaces and large molecules. The adaptive local basis functions are non-polynomial basis functions, and standard a posteriori error estimates for $hp$-refinement using polynomial basis functions do not directly apply. We generalize the error estimates for $hp$-refinement to non-polynomial basis functions. We demonstrate the practical use of the a posteriori error estimator in performing three-dimensional Kohn-Sham density functional theory calculations for quasi-2D aluminum surfaces and a single-layer graphene oxide system in water.