Atomistic theory of twist-angle dependent intralayer and interlayer exciton properties in twisted bilayer materials

Twisted bilayers of two-dimensional (2D) materials have emerged as a highly tunable platform to study and engineer properties of excitons. However, the atomistic description of these properties has remained a significant challenge as a consequence of the large unit cells of the emergent moir\'e superlattices. To address this problem, we introduce an efficient approach to solve the Bethe-Salpeter equation that exploits the localization of atomic Wannier functions. We then use this approach to study intra- and interlayer excitons in twisted WS₂/WSe₂ at a range of twist angles. In agreement with experiment, we find that the optical spectrum exhibits three low-energy peaks for twist angles small than 2^∘. The energy splitting between the peaks is described accurately. We also find two low-energy interlayer excitons with weak oscillator strengths. Our approach opens up new opportunities for the design of light-matter interactions in ultrathin materials.