Screening and many-body effects in two-dimensional crystals: Monolayer<mml:math xmlns:mml="http://www.w3.org/1998/Math/MathML"><mml:msub><mml:mi>MoS</mml:mi><mml:mn>2</mml:mn></mml:msub></mml:math>

Abstract

We present a systematic study of the variables affecting the electronic and optical properties of two-dimensional (2D) crystals within ab initio $GW$ and $GW$ plus Bethe-Salpeter equation ($GW$-BSE) calculations. As a prototypical 2D transition metal dichalcogenide material, we focus our study on monolayer ${\mathrm{MoS}}_{2}$. We find that the reported variations in $GW$-BSE results in the literature for monolayer ${\mathrm{MoS}}_{2}$ and related systems arise from different treatments of the long-range Coulomb interaction in supercell calculations and convergence of $k$-grid sampling and cutoffs for various quantities such as the dielectric screening. In particular, the quasi-2D nature of the system gives rise to fast spatial variations in the screening environment, which are computationally challenging to resolve. We also show that common numerical treatments to remove the divergence in the Coulomb interaction can shift the exciton continuum leading to false convergence with respect to $k$-point sampling. Our findings apply to $GW$-BSE calculations on any low-dimensional semiconductors.