$G^0W^0$ implementation based on the pseudopotential and numerical-atomic-orbital basis-set framework: Algorithms and benchmarks

TL;DR

This paper introduces an efficient $G^0W^0$ computational framework based on the NAO-PP scheme, combining novel algorithms and benchmarks to improve accuracy and efficiency in electronic structure calculations.

Contribution

The work presents a new NAO-PP-based $G^0W^0$ implementation with innovative compression and dielectric treatment techniques, validated through systematic benchmarks.

Findings

High accuracy in band structure and gap calculations.

Significant computational efficiency improvements.

Excellent agreement with established $G^0W^0$ methods.

Abstract

The $GW$ method delivers substantially improved accuracy in electronic band structure calculations over conventional Kohn-Sham density functional theory (KS-DFT) by explicitly incorporating the electron self-energy effect beyond mean-field approximations. Despite many existing implementations, a periodic $GW$ implementation within the framework of numerical atomic orbitals (NAO) combined with the pseudopotential (PP) scheme has not been reported. This is urgently needed given the increasing popularity of the NAO-PP framework in KS-DFT calculations and its importance for the development of machine-learning electronic-structure approaches. In this work, we present an efficient NAO-PP-based $G^0W^0$ computational framework by interfacing the first-principles software package ABACUS with LibRPA -- a library for performing low-scaling random-phase approximation and $GW$ calculations based on NAOs. Our approach employs the localized resolution of identity (LRI) technique with a novel compression scheme, significantly improving both computational efficiency and numerical stability. In addition, an analytic treatment of the small-q limit of the microscopic dielectric function reduces the need for dense q-point sampling. Furthermore, we propose a practical strategy to select a suitable KS-DFT pseudopotential prior to $G^0W^0$ calculations by examining the frequency-dependent macroscopic dielectric function. Systematic benchmarks validate the effectiveness of our compression scheme and real-space tensor filtering strategies, demonstrating both high accuracy and significant computational efficiency gains. Comparisons with established $G^0W^0$ implementations show excellent agreement in band structures and band gaps, confirming ABACUS+LibRPA as a reliable and efficient platform for large-scale $G^0W^0$ simulations.