All-electron self-consistent GW in the Matsubara-time domain: implementation and benchmarks of semiconductors and insulators

TL;DR

This paper presents an efficient all-electron GW implementation in the Matsubara-time domain, benchmarking its accuracy on semiconductors and insulators, and comparing analytic continuation methods for electronic structure calculations.

Contribution

It introduces a computationally efficient Matsubara-time GW approach with a new analytic continuation method and benchmarks it against experimental data for various materials.

Findings

G0W0 matches experiments for simple s-p systems

scGW improves band gaps in 3-d electron systems

CPE and Pade give similar results for most materials

Abstract

The GW approximation is a well-known method to improve electronic structure predictions calculated within density functional theory. In this work, we have implemented a computationally efficient GW approach that calculates central properties within the Matsubara-time domain using the modified version of Elk, the full-potential linearized augmented plane wave (FP-LAPW) package. Continuous-pole expansion (CPE), a recently proposed analytic continuation method, has been incorporated and compared to the widely used Pade approximation. Full crystal symmetry has been employed for computational speedup. We have applied our approach to 18 well-studied semiconductors/insulators that cover a wide range of band gaps computed at the levels of single-shot G0W0, partially self-consistent GW0, and fully self-consistent GW (scGW). Our calculations show that G0W0 leads to band gaps that agree well with experiment for the case of simple s-p electron systems, whereas scGW is required for improving the band gaps in 3-d electron systems. In addition, GW0 almost always predicts larger band gap values compared to scGW, likely due to the substantial underestimation of screening effects. Both the CPE method and Pade approximation lead to similar band gaps for most systems except strontium titantate, suggesting further investigation into the latter approximation is necessary for strongly correlated systems. Our computed band gaps serve as important benchmarks for the accuracy of the Matsubara-time GW approach.