All-electron BSE@GW method with Numeric Atom-Centered Orbitals for Extended Systems

TL;DR

This paper introduces a new all-electron BSE@GW computational method using numeric atom-centered orbitals, optimized for extended periodic systems, with demonstrated accuracy and convergence testing.

Contribution

It presents the implementation of an all-electron BSE@GW approach for extended systems with periodic boundary conditions using numeric atom-centered orbitals.

Findings

Successful implementation for extended systems with periodic boundary conditions.

Convergence tests show reliable results with various basis sets.

Comparison with other formalisms validates the new method.

Abstract

Green's function theory has emerged as a powerful many-body approach not only in condensed matter physics but also in quantum chemistry in recent years. We have developed a new all-electron implementation of the BSE@GW formalism using numeric atom-centered orbital basis sets (Liu et al., J. Chem. Phys. 152, 044105 (2020)). We present our recent developments in implementing this formalism for extended systems with periodic boundary conditions. We discuss its numerical implementation and various convergence tests pertaining to numerical atom-centered orbitals, auxiliary basis sets for the resolution-of-identity formalism, and Brillouin zone sampling. Proof-of-principle examples are presented to compare with other formalisms, illustrating the new all-electron BSE@GW method for extended systems.