Real space representation of the quasiparticle self-consistent $GW$ self-energy and its application to defect calculations

TL;DR

This paper develops a real space representation of the quasiparticle self-consistent GW self-energy, enabling efficient defect calculations by combining parts of the system, and demonstrates its accuracy on GaAs defect states.

Contribution

It introduces a real space, atom-centered basis set approach to the QS$GW$ self-energy, facilitating scalable defect calculations by a cut-and-paste method.

Findings

The self-energy is short-ranged, enabling localized defect modeling.

The method accurately reproduces defect levels in GaAs compared to direct calculations.

It allows efficient construction of defect self-energies from smaller system calculations.

Abstract

The quasiparticle self-consistent QS$GW$ approach incorporates the corrections of the quasiparticle energies from their Kohn-Sham density functional theory (DFT) eigenvalues by means of an energy independent and Hermitian self-energy matrix usually given in the basis set of the DFT eigenstates. By expanding these into an atom-centered basis set (specifically here the linearized muffin-tin orbitals) a real space representation of the self-energy corrections becomes possible. We show that this representation is relatively short-ranged. This offers new opportunities to construct the self-energy of a complex system from parts of the system by a cut-and-paste method. Specifically for a point defect, represented in a large supercell, the self-eneregy can be constructed from those of the host and a smaller defect containing cell. The self-energy of the periodic host can be constructed simply from a $GW$ calculation for the primitive cell. We show for the case of the As$_\mathrm{Ga}$ in GaAs that the defect part can already be well represented by a minimal 8 atom cell and allows us to construct the self-energy for a 64 cell in good agreement with direct QS$GW$ calculations for the large cell. Using this approach to an even larger 216 atom cell shows the defect band approaches an isolated defect level. The calculations also allow to identify a second defect band which appears as a resonance near the conduction band minimum. The results on the extracted defect levels agree well with Green's function calculations for an isolated defect and with experimental data.