Excitons in two-dimensional atomic layer materials from time-dependent density functional theory

Abstract: Time-dependent density functional theory (TDDFT) has been applied to the calculation of absorption spectra for two-dimensional atomic layer materials. We reveal that the character of the first bright exciton state of bi-layer hexagonal boron nitride (h-BN) is dependent on the layer stacking type through the use of many-body perturbation theory (MBPT) calculations, i.e., the electron and hole in the AA$'$ stacking are present in the same layer (intralayer exciton) while the A$'$B stacking exhibits an interlayer exciton. We demonstrate that the TDDFT approach with the meta-generalized gradient approximation to the exchange-correlation (XC) potential, and the Bootstrap XC kernel can capture the absorption peaks that correspond to these excitons without computationally heavy GW and Bethe-Salpeter equation calculations. We also show that the TDDFT method provides the absorption spectra for mono-layer transition metal dichalcogenides, MoS$_2$ and MoSe$_2$. This study confirms the validity of the TDDFT approach for the first investigation of the optical properties of complex two-dimensional atomic layer materials to which the MBPT calculation can not be readily applied.