Ferroelectric-Driven Exciton and Trion Modulation in Monolayer Molybdenum and Tungsten Diselenides

In this work, we show how domain-engineered lithium niobate can be used to selectively dope monolayer molybdenum selenide (MoSe₂) and tungsten selenide (WSe₂) and demonstrate that these ferroelectric domains can significantly enhance or inhibit photoluminescence (PL), with the most dramatic modulation occurring at the heterojunction interface between two domains. A micro-PL and Raman system is used to obtain spatially resolved images of the differently doped transition metal dichalcogenides (TMDs). The domain-inverted lithium niobate causes changes in the TMDs due to electrostatic doping as a result of the remnant polarization from the substrate. Moreover, the differently doped TMDs (n-type MoSe₂ and p-type WSe₂) exhibit opposite PL modulation. Distinct oppositely charged domains were obtained with a 9-fold PL enhancement for the same single MoSe₂ sheet when adhered to the positive (P⁺) and negative (P^-) domains. This sharp PL modulation on the ferroelectric domain results from different free electron or hole concentrations in the material's conduction band or valence band. Moreover, excitons dissociate rapidly at the interface between the P⁺ and P^- domains due to the built-in electric field. We are able to adjust the charge on the P⁺ and P^- domains using temperature via the pyroelectric effect and observe rapid PL quenching over a narrow temperature range, illustrating the observed PL modulation is electronic in nature. This observation creates an opportunity to harness the direct bandgap TMD 2D materials as an active optical component for the lithium niobate platform using domain engineering of the lithium niobate substrate to create optically active heterostructures that could be used for photodetectors or even electrically driven optical sources on-chip.