Critical assessment of $G_0{W}_0$ calculations for 2D materials: the example of monolayer MoS${}_2$

Abstract

Two-dimensional (2D) materials combine many fascinating properties that make them more interesting than their three-dimensional counterparts for a variety of applications. For example, 2D materials exhibit stronger electron-phonon and electron-hole interactions, and their energy gaps and effective carrier masses can be easily tuned. Surprisingly, published band gaps of several 2D materials obtained with the $GW$ approach, the state-of-the-art in electronic-structure calculations, are quite scattered. The details of these calculations, such as the underlying geometry, the starting point, the inclusion of spin-orbit coupling, and the treatment of the Coulomb potential can critically determine how accurate the results are. Taking monolayer MoS${}_2$ as a representative material, we employ the linearized augmented planewave + local orbital method to systematically investigate how all these aspects affect the quality of $G_0{W}_0$ calculations, and also provide a summary of literature data. We conclude that the best overall agreement with experiments and coupled-cluster calculations is found for $G_0{W}_0$ results with HSE06 as a starting point including spin-orbit coupling, a truncated Coulomb potential, and an analytical treatment of the singularity at $q=0$.

arXiv commentThis version of the article has been accepted for publication, after peer review but is not the Version of Record and does not reflect post-acceptance improvements, or any corrections. The Version of Record is available online at: http://dx.doi.org/10.1038/s41524-024-01253-2

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Cited by in corpus (3)

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• Quasiparticle and fully self-consistent GW methods: an unbiased analysis using Gaussian orbitals
• Efficient $GW$ band structure calculations using Gaussian basis functions and application to atomically thin transition-metal dichalcogenides