Renormalized Singles Green's Function for Quasi-Particle Calculations beyond the G0 W0 Approximation.

Abstract

Quasi-particle energies and band gaps in particular are critical for investigating novel materials. Commonly used density functional approximations (DFAs) systematically underestimate band gaps, and GW approximation is the established method of choice for good accuracy and reliability. However, G0 W0 has some undesired dependence on the DFA, while self-consistent GW (sc GW) is expensive and not consistent in accuracy improvement. Here a simple and efficient GRS W0 approach has been developed: a subspace diagonalization of the Hartree-Fock (HF) Hamiltonian with the DFA density matrix provides the new reference Green's function GRS that incorporates the effect of all single excitation contributions to the self-energy, thereby essentially eliminating the starting-point dependence. Calculations for molecules and large band gap solids demonstrate the significant improvement over G0 W0 and greatly reduced dependence on the initial DFA. GRS W0 approach also improve results for other bulks over G0 W0, but to a lesser extent, which could be due to the limitations in current implementation for bulks. The results demonstrate that to achieve good accuracy, it is not necessary to use hybrid DFA, which is expensive for bulks. This work should be greatly significant in making GW a more robust approach.