Spinor GW/Bethe-Salpeter calculations in BerkeleyGW: Implementation, symmetries, benchmarking, and performance

Bradford A. Barker, Jack Deslippe, Johannes Lischner, Manish Jain, Oleg V. Yazyev, David A. Strubbe, and Steven G. Louie
Phys. Rev. B 106, 115127 – Published 15 September 2022
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Abstract

Computing the GW quasiparticle band structure and Bethe-Salpeter equation (BSE) absorption spectra for materials with spin-orbit coupling have commonly been done by treating GW corrections and spin-orbit coupling (SOC) as separate perturbations to density-functional theory. However, accurate treatment of materials with strong spin-orbit coupling (such as many topological materials of recent interest, and thermoelectrics) often requires a nonperturbative approach using spinor wave functions in the Kohn-Sham equation and GW/BSE. Such calculations have only recently become available, in particular for the BSE. We have implemented this approach in the plane-wave pseudopotential GW/BSE code BerkeleyGW, which is highly parallelized and widely used in the electronic-structure community. We present reference results for quasiparticle band structures and optical absorption spectra of solids with different strengths of spin-orbit coupling, including Si, Ge, GaAs, GaSb, CdSe, Au, and Bi2Se3. The calculated quasiparticle band gaps of these systems are found to agree with experiment to within a few tens of meV. SOC splittings are found to be generally in better agreement with experiment, including quasiparticle corrections to band energies. The absorption spectrum of GaAs is not significantly impacted by the inclusion of spin-orbit coupling due to its relatively small value (0.2 eV) in the Λ direction, while the absorption spectrum of GaSb calculated with the spinor GW/BSE captures the large spin-orbit splitting of peaks in the spectrum. For the prototypical topological insulator Bi2Se3, we find a drastic change in the low-energy band structure compared to that of DFT, with the spinorial treatment of the GW approximation correctly capturing the parabolic nature of the valence and conduction bands after including off-diagonal self-energy matrix elements. We present the detailed methodology, approach to spatial symmetries for spinors, comparison against other codes, and performance compared to spinless GW/BSE calculations and perturbative approaches to SOC. This work aims to spur further development of spinor GW/BSE methodology in excited-state research software and enables a more accurate and detailed exploration of electronic and optical properties of materials containing elements with large atomic numbers.

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  • Received 28 May 2022
  • Revised 25 August 2022
  • Accepted 6 September 2022

DOI:https://doi.org/10.1103/PhysRevB.106.115127

©2022 American Physical Society

Physics Subject Headings (PhySH)

Condensed Matter, Materials & Applied Physics

Authors & Affiliations

Bradford A. Barker1,2,3,*, Jack Deslippe4, Johannes Lischner5, Manish Jain6, Oleg V. Yazyev7, David A. Strubbe3, and Steven G. Louie1,2

  • 1Department of Physics, University of California, Berkeley, Berkeley, California 94720, USA
  • 2Materials Sciences Division, Lawrence Berkeley National Laboratory, Berkeley, California 94720, USA
  • 3Department of Physics, University of California, Merced, Merced, California 95343, USA
  • 4National Energy Research Scientific Computing Center, Lawrence Berkeley National Laboratory, Berkeley, California 94720, USA
  • 5Department of Materials and Physics, and Thomas Young Centre for Theory and Simulation of Materials, Imperial College London, London SW7 2AZ, United Kingdom
  • 6Center for Condensed Matter Theory, Department of Physics, Indian Institute of Science, Bangalore 560012, India
  • 7Institute of Physics, Ecole Polytechnique Federale de Lausanne (EPFL), CH-1015 Lausanne, Switzerland

  • *bbarker6@ucmerced.edu

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Issue

Vol. 106, Iss. 11 — 15 September 2022

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