Identification of Exciton Complexes in Charge-Tunable Janus WSeS Monolayers.

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 WSeS monolayers with ∼6 meV optical line widths. We integrate Janus monolayers into vertical heterostructures, allowing doping control. Magneto-optic measurements indicate that monolayer WSeS 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.

Room-Temperature Synthesis of 2D Janus Crystals and their Heterostructures.

Janus crystals represent an exciting class of 2D materials with different atomic species on their upper and lower facets. Theories have predicted that this symmetry breaking induces an electric field and leads to a wealth of novel properties, such as large Rashba spin-orbit coupling and formation of strongly correlated electronic states. Monolayer MoSSe Janus crystals have been synthesized by two methods, via controlled sulfurization of monolayer MoSe2 and via plasma stripping followed thermal annealing of MoS2 . However, the high processing temperatures prevent growth of other Janus materials and their heterostructures. Here, a room-temperature technique for the synthesis of a variety of Janus monolayers with high structural and optical quality is reported. This process involves low-energy reactive radical precursors, which enables selective removal and replacement of the uppermost chalcogen layer, thus transforming classical transition metal dichalcogenides into a Janus structure. The resulting materials show clear mixed character for their excitonic transitions, and more importantly, the presented room-temperature method enables the demonstration of first vertical and lateral heterojunctions of 2D Janus TMDs. The results present significant and pioneering advances in the synthesis of new classes of 2D materials, and pave the way for the creation of heterostructures from 2D Janus layers.