Cubic-scaling all-electron GW calculations with a separable density-fitting space-time approach

Abstract

We present an implementation of the $GW$ space-time approach that allows cubic-scaling all-electron calculations with standard Gaussian basis sets without exploiting any localization nor sparsity considerations. The independent-electron susceptibility is constructed in a time representation over a non-uniform distribution of real-space locations $\{{\mathbf{r}}_k\}$ optimized within a separable resolution-of-the-identity framework to reproduce standard Coulomb-fitting calculations with meV accuracy. The compactness of the obtained $\{{\mathbf{r}}_k\}$ distribution leads to a crossover with the standard Coulomb-fitting scheme for system sizes below a few hundred electrons. The needed analytic continuation follows a recent approach that requires the continuation of the screened Coulomb potential rather than the much more structured self-energy. The present scheme is benchmarked over large molecular sets and scaling properties are demonstrated on a family of defected hexagonal boron-nitride flakes containing up to 6000 electrons.