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.

Low-temperature synthesis of 2D anisotropic MoTe2 using a high-pressure soft sputtering technique.

We demonstrate a high-pressure soft sputtering technique that can grow large area 1T' phase MoTe2 sheets on HOPG and Al2O3 substrates at temperatures as low as 300 °C. The results show that a single Mo/Te co-sputtering step on heated substrates produces highly defected films as a result of the low Te sticking coefficient. The stoichiometry is significantly improved when a 2-step technique is used, which first co-sputters Mo and Te onto an unheated substrate and then anneals the deposited material to crystalize it into 1T' phase MoTe2. A MoTe2-x 1T' film with the lowest Te vacancy content (x = 0.14) was synthesized using a 300 °C annealing step, but a higher processing temperature was prohibited due to MoTe2 decomposition with an activation energy of 80.7 kJ mol-1. However, additional ex situ thermal processing at ∼1 torr tellurium pressure can further reduce the Te-vacancy (VTe) concentration, resulting in an improvement in the composition from MoTe1.86 to MoTe1.9. Hall measurements indicate that the films produced with the 2-step in situ process are n-type with a carrier concentration of 4.6 × 1014 cm-2 per layer, presumably from the large VTe concentration stabilizing the 1T' over the 2H phase. Our findings (a) demonstrate that large scale synthesis of tellurium based vdW materials is possible using industrial growth and processing techniques and (b) accentuate the challenges in producing stoichiometric MoTe2 thin films.