Efficient electrical switching of exciton states for valley contrast manipulation in two-dimensional perovskite/monolayer WS2 heterostructures

Abstract: The coupled spin-valley physics in transition metal dichalcogenides (TMDs) endows exciton states with valley degrees of freedom, making them promising for valleytronic applications in TMDs monolayers and/or their heterostructures. Although the valley dynamics of intralayer and interlayer excitons (IXs) have been studied, efficient manipulation of valley pseudospins by switching exciton states remains elusive. Therefore, it is of great importance to effectively tune the exciton states to obtain practical valley polarization switches for valley encoding. Here, we demonstrate the electrical switching of exciton emission with highly variable valley polarization mediated by charged IXs (CIXs) in the heterostructure of monolayer WS2 and two-dimensional (2D) perovskite, irrespective of lattice constants, the rotational and translational alignment. The formation of IXs is identified by photoluminescence excitation (PLE) and photoluminescence (PL) studies, which can be further electrically tuned from positively charged to negatively charged depending on the electrostatic doping level of monolayer WS2. Importantly, we demonstrate an electrical switching from type two to type one band alignment, manifesting as a change in the PL profile from CIX to charged intralayer exciton emission. Such transition induces a large contrast in valley polarization between the two exciton states, enabling the reversible electrically regulated valley polarization switch with a maximum ON/OFF ratio of 15.8. Our study provides an alternative mechanism to achieve valley polarization switching with great simplicity for valleytronics and the electrical control of exciton species and associated valley-contrasting physics would further facilitate the development of optoelectronic and valleytronic devices