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Monolayer (ML) transition metal dichalcogenides (TMDs) undergo substantialchanges in the single-particle band structure and excitonic optical responseupon the addition of just one layer. As opposed to the single-layer limit, thebandgap of bilayer (BL) TMD semiconductors is indirect which results in reducedphotoluminescence with richly structured spectra that have eluded a detailedunderstanding to date. Here, we provide a closed interpretation of theelementary optical responses of BL WSe$_2$ as a representative material for thewider class of TMD semiconductors. By combining theoretical calculations withcomprehensive spectroscopy experiments, we identify the crucial role ofmomentum-indirect excitons for the understanding of basic absorption andemission spectra ubiquitously exhibited by various TMD BLs. Our results shedlight on the origin of quantum dot (QD) formation in monolayer and bilayercrystals and will facilitate further advances directed at opto-electronicapplications of layered TMD semiconductors in van der Waals heterostructuresand devices.

The role of momentum-dark excitons in the elementary optical response of bilayer WSe$_{2}$