We describe an all-electron GW implementation for periodic systems with k-point sampling using a crystalline Gaussian basis. Due to the compactness of Gaussian bases, no virtual state truncation is required as is seen in many plane-wave formulations. Using our implementation, we study quasiparticle energies and band structures across a range of systems including semiconductors, rare gas solids, and metals. We find that the G0W0 band gaps of traditional semiconductors converge rapidly with respect to the basis size, even for the conventionally challenging case of ZnO. Using correlation-consistent bases of polarized triple-zeta quality, we find the mean absolute relative error of the extrapolated G0W0@PBE band gaps to be only 5.2% when compared to experimental values. For core excitation binding energies, we find that G0W0 predictions improve significantly over those from DFT, especially when the G0W0 calculations are started from hybrid functionals with a high percentage of exact exchange.

All-electron Gaussian-based GW methods for periodic systems

ACS Fall 2021

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