Renormalized Singles Green's Function in the T-Matrix Approximation for Accurate Quasiparticle Energy Calculation.

We combine the renormalized singles (RS) Green's function with the T-matrix approximation for the single-particle Green's function to compute quasiparticle energies for valence and core states of molecular systems. The method uses the RS Green's function that incorporates singles contributions as the initial Green's function. The method further calculates the generalized effective interaction with the RS Green's function by using RS eigenvalues in the T-matrix calculation through the particle-particle random phase approximation. The method provides significant improvements over one-shot methods and as demonstrated in calculations for GW100 and CORE65 test sets. It also systematically eliminates the dependence of on the choice of density functional approximations. For valence states, the method provides excellent accuracy, which is better than that of and . For core states, the method identifies correct peaks in the spectral function and significantly outperforms on core-level binding energies (CLBEs) and relative CLBEs.