Cubic-Scaling All-Electron GW Calculations with a Separable Density-Fitting Space-Time Approach

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 or sparsity considerations. The independent-electron susceptibility is constructed in a time representation over a nonuniform distribution of real-space locations {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 {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.

Automated summary

The study presents an implementation of the GW space-time approach for cubic-scaling all-electron calculations with standard Gaussian basis sets without localization or sparsity considerations. The method is benchmarked on large molecular sets and demonstrates scaling properties on a family of defected hexagonal boron-nitride flakes.