Phonon‐Induced Markovian and Non‐Markovian Effects on Absorption Spectra of Moiré Excitons in Twisted Transition Metal Dichalcogenide Bilayers

ABSTRACT The properties of moiré excitons in twisted bilayers of transition metal dichalcogenides (TMDCs) vary significantly with the twist angle, ranging from quasi‐localized excitons with flat dispersions for small twist angles to delocalized excitons for larger ones. This twist‐angle dependence directly impacts the exciton–phonon coupling, which plays a significant role for the optical properties of these materials. In this work, we theoretically investigate the twist‐angle‐dependent influence of phonons on absorption spectra of intralayer moiré excitons in a twisted TMDC heterobilayer. For the lowest‐lying intralayer moiré exciton, we find that the exciton–phonon coupling interpolates between two physically distinct regimes when tuning the twist angle. At small twist angles non‐Markovian polarization dynamics and phonon sidebands dominate the properties of absorption spectra for localized excitons. For larger twist angles Markovian processes become more important, leading to additional line broadening. Furthermore, the absorption spectra here show a characteristic asymmetric peak similar to monolayer TMDCs. When taking into account multiple bright moiré exciton bands, we find that intraband scattering due to optical phonons has a significant impact on absorption spectra, effectively suppressing absorption peaks of higher lying bands when their bandwidth surpasses the optical phonon energy.