Renormalized Singles with Correlation in GW Green's Function Theory for Accurate Quasiparticle Energies.

We apply the renormalized singles with the correlation (RSc) Green function in the GW approximation for accurate quasiparticle (QP) energies and orbitals. The RSc Green function includes singles contributions from the associated density functional approximation (DFA) and considers correlation contributions perturbatively. G_RScW_RSc uses the RSc Green function as the new starting point and in the formulation of the screened interaction. G_RScW₀ fixes the screened interaction at the DFA level. For the calculations of ionization potentials, G_RScW_RSc and G_RScW₀ significantly reduce the starting point dependence and provide accurate results with errors around 0.2  eV. For the calculations of core-level binding energies, G_RScW_RSc slightly overestimates the results because of underscreening, but G_RScW₀ with GGA functionals provides the optimal accuracy with errors of 0.40  eV. We also show that G_RScW_RSc predicts accurate dipole moments. G_RScW_RSc and G_RScW₀, are computationally favorable compared with any self-consistent GW methods. The RSc approach is promising for making GW and other Green function methods efficient and robust.

Duke Scholars

Author Weitao Yang Chemistry