Identification of Exciton Complexes in Charge-Tunable Janus W(Se)(S) Monolayers

[Image: see text] Janus transition-metal dichalcogenide monolayers are artificial materials, where one plane of chalcogen atoms is replaced by chalcogen atoms of a different type. Theory predicts an in-built out-of-plane electric field, giving rise to long-lived, dipolar excitons, while preserving direct-bandgap optical transitions in a uniform potential landscape. Previous Janus studies had broad photoluminescence (>18 meV) spectra obfuscating their specific excitonic origin. Here, we identify the neutral and the negatively charged inter- and intravalley exciton transitions in Janus W(Se)(S) monolayers with ∼6 meV optical line widths. We integrate Janus monolayers into vertical heterostructures, allowing doping control. Magneto-optic measurements indicate that monolayer W(Se)(S) has a direct bandgap at the K points. Our results pave the way for applications such as nanoscale sensing, which relies on resolving excitonic energy shifts, and the development of Janus-based optoelectronic devices, which requires charge-state control and integration into vertical heterostructures.