New JCTC paper from Tomi Ketolainen, Nikola Macháčová and František Karlický

Optical Gaps and Excitonic Properties of 2D Materials by Hybrid TD-DFT: Evidences for Monolayers and Prospects for vdW Heterostructures
(ACS)

Tomi Ketolainen, Nikola Macháčová, and František Karlický

Abstract

The optical properties of two-dimensional (2D) materials are accurately described by many-body methods including specifically pronounced electron-electron and electron-hole effects. Such methods are, however, computationally demanding and applicable on small computational cells only. We provide approximate optical gaps for 2D materials from time dependent density functional theory (TD-DFT) based on a set of specific screened hybrid functionals and show that this approach effectively accounts for all important physical effects including excitons. Optical gap values obtained from the TD-HSE06 approach for a broad gap range 1 – 6 eV of eight 2D materials are in agreement with both experimental optical gaps and accurate GW+BSE calculations. Further, we show that such an approach is eligible and practicable for van der Waals heterostructures containing incommensurate cells of different monolayers and enables detailed analysis of intra- and inter-layer excitonic wave functions. TD-HSE06 is therefore a suitable method for a reliable description of the optical properties of extended periodic 2D systems.