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Optimally tuned starting point for single-shot <mml:math xmlns:mml="http://www.w3.org/1998/Math/MathML"><mml:mrow><mml:mi>G</mml:mi><mml:mi>W</mml:mi></mml:mrow></mml:math> calculations of solids

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

2022Physical Review Materials38 citationsDOIOpen Access PDF

Abstract

The dependence of ab initio many-body perturbation theory within the $GW$ 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 $GW$ (${G}_{0}{W}_{0}$) 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 $GW$ 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 $GW$ and eigenvalue self-consistent $GW$. 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.

Topics & Concepts

QuasiparticleAb initioValence (chemistry)PhysicsEigenvalues and eigenvectorsAlgorithmCondensed matter physicsQuantum mechanicsMathematicsSuperconductivityAdvanced Chemical Physics StudiesPhysics of Superconductivity and MagnetismMachine Learning in Materials Science
Optimally tuned starting point for single-shot <mml:math xmlns:mml="http://www.w3.org/1998/Math/MathML"><mml:mrow><mml:mi>G</mml:mi><mml:mi>W</mml:mi></mml:mrow></mml:math> calculations of solids | Litcius