Computing the self-consistent field in Kohn–Sham density functional theory

Abstract

Abstract A new framework is presented for evaluating the performance of self-consistent field methods in Kohn–Sham density functional theory (DFT). The aims of this work are two-fold. First, we explore the properties of Kohn–Sham DFT as it pertains to the convergence of self-consistent field iterations. Sources of inefficiencies and instabilities are identified, and methods to mitigate these difficulties are discussed. Second, we introduce a framework to assess the relative utility of algorithms in the present context, comprising a representative benchmark suite of over fifty Kohn–Sham simulation inputs, the scf-x n suite. This provides a new tool to develop, evaluate and compare new algorithms in a fair, well-defined and transparent manner.