GW calculations on post-transition-metal oxides

Abstract

In order to establish the reliable GW scheme that can be consistently applied to post-transition-metal oxides (post-TMOs), we carry out comprehensive GW calculations on electronic structures of ZnO, Ga2O3, In2O3, and SnO2, the four representative post-TMOs. Various levels of self-consistency (G(0)W(0), GW(0), and QPGW(0)) and different starting functionals (GGA, GGA + U, and hybrid functional) are tested and their influence on the resulting electronic structure is closely analyzed. It is found that the GW0 scheme with GGA + U as the initial functional turns out to give the best agreement with experiment, implying that describing the position of metal-d level precisely in the ground state plays a critical role for the accurate dielectric property and quasiparticle band gap. Nevertheless, the computation on ZnO still suffers from the shallow Zn-d level and we propose a modified approach (GW(0) + U-d) that additionally considers an effective Hubbard U term during GW0 iterations and thereby significantly improves the band gap. It is also shown that a GGA + U-based GW0(+ Ud) scheme produces an accurate energy gap of crystalline InGaZnO4, implying that this can serve as a standard scheme that can be applied to general structures of post-TMOs.