Optimally tuned starting point for single-shot $GW$ calculations of solids

Optimally tuned starting point for single-shot $G W$ calculations of solids

Stephen E. Gant, Jonah B. Haber, Marina R. Filip, Francisca Sagredo, Dahvyd Wing, Guy Ohad, Leeor Kronik, and Jeffrey B. Neaton

Phys. Rev. Materials 6, 053802 – Published 16 May 2022

Abstract

The dependence of ab initio many-body perturbation theory within the $G W$ approximation on the eigensystem used in calculating quasiparticle corrections limits this method's predictive power. Here, we investigate the accuracy of the recently developed Wannier-localized optimally tuned screened range-separated hybrid (WOT-SRSH) functional as a generalized Kohn-Sham starting point for single-shot $G W$ ( $G_{0} W_{0}$ ) calculations for a range of semiconductors and insulators. Comparison to calculations based on well-established functionals, namely, PBE, PBE0, and HSE, as well as to self-consistent $G W$ schemes and to experiment, shows that band gaps computed via $G_{0} W_{0}$ @WOT-SRSH have a level of precision and accuracy that is comparable to that of more advanced methods such as quasiparticle self-consistent $G W$ and eigenvalue self-consistent $G W$ . We also find that $G_{0} W_{0}$ @WOT-SRSH improves the description of states deeper in the valence band manifold. Finally, we show that $G_{0} W_{0}$ @WOT-SRSH significantly reduces the sensitivity of computed band gaps to ambiguities in the underlying WOT-SRSH tuning procedure.

Received 28 January 2022
Accepted 6 April 2022

DOI:https://doi.org/10.1103/PhysRevMaterials.6.053802

Physics Subject Headings (PhySH)

Electronic structure First-principles calculations

Crystalline systems Insulators Semiconductors

Density functional theory GW method Hybrid functionals

Condensed Matter, Materials & Applied PhysicsEnergy Science & Technology

Authors & Affiliations

Stephen E. Gant ¹, Jonah B. Haber¹, Marina R. Filip², Francisca Sagredo ¹, Dahvyd Wing³, Guy Ohad ³, Leeor Kronik³, and Jeffrey B. Neaton^1,4,5,*

¹Department of Physics, University of California Berkeley, Berkeley, California 94720, USA
²Department of Physics, University of Oxford, Clarendon Laboratory, Oxford OX1 3PU, England, United Kingdom
³Department of Molecular Chemistry and Materials Science, Weizmann Institute of Science, Rehovoth 76100, Israel
⁴Materials Sciences Division, Lawrence Berkeley National Laboratory, Berkeley, California 94720, USA
⁵Kavli Energy NanoScience Institute at Berkeley, Berkeley, California 94720, USA