Neutral and charged excitons (trions) in atomically thin materials offer important capabilities for photonics, from ultrafast photodetectors to highly efficient light-emitting diodes and lasers. Recent studies of van der Waals (vdW) heterostructures comprised of dissimilar monolayer materials have uncovered a wealth of optical phenomena that are predominantly governed by interlayer interactions. Here, we examine the optical properties in NbSe2-MoSe2 vdW heterostructures, which provide an important model system to study metal-semiconductor interfaces, a common element in optoelectronics. Through low-temperature photoluminescence (PL) microscopy, we discover a sharp emission feature, L1, that is localized at the NbSe2-capped regions of MoSe2. L1 is observed at energies below the commonly studied MoSe2 excitons and trions and exhibits temperature- and power-dependent PL consistent with exciton localization in a confining potential. This PL feature is robust, observed in a variety of samples fabricated with different stacking geometries and cleaning procedures. Using first-principles calculations, we reveal that the confinement potential required for exciton localization naturally arises from the in-plane band bending due to the changes in the electron affinity between pristine MoSe2 and NbSe2-MoSe2 heterostructure. We discuss the implications of our studies for atomically thin optoelectronics devices with atomically sharp interfaces and tunable electronic structures.
Keywords: density functional theory; excitons; photoluminescence; transition metal dichalcogenides; van der Waals heterostructures.