Extrinsic localized excitons in patterned 2D semiconductors

Abstract

We demonstrate a new localized excitonic state in patterned monolayer 2D semiconductors. This state is not associated with lattice disorder but is extrinsic, i.e. results from external molecules on the material surface. The signature of an exciton associated with that state is observed in the photoluminescence spectrum after electron beam exposure of several 2D semiconductors. The localized state, which is distinguished by non-linear power dependence, survives up to room temperature and is patternable down to 20 nm resolution. We probe the response of the new exciton to the changes of electron energy, nanomechanical cleaning, and encapsulation via multiple microscopic, spectroscopic, and computational techniques. All these approaches suggest that the state does not originate from irradiation-induced structural defects or spatially non-uniform strain, as commonly assumed. Instead, we show that it is extrinsic, likely a charge transfer exciton associated with the organic substance deposited onto the 2D semiconductor. By demonstrating that structural defects are not required for the formation of localized excitons, our work opens new possibilities for further understanding of these states and using them for example in chemical sensing and quantum technologies.