Near-field exciton imaging of chemically treated MoS2 monolayers

Abstract

The exciton-dominated light emission of two-dimensional (2D) semiconductors is determined largely by the doping state and the formation of defects. Extensive studies have shown that chemical treatment critically modifies the doping state and defect state of chemical vapor deposition (CVD)-grown or exfoliated monolayer MoS₂ (1L-MoS₂), suggesting a promising possibility for engineering the optoelectronic properties of 2D semiconductors. However, chemical treatment inevitably modifies both the doping state and defect states, and their independent roles in the exciton emission of 1L-MoS₂ have been difficult to study, significantly limiting the practical and reliable uses of chemical treatment to improve the optical properties of 1L-TMDs. Herein, we used near-field imaging and spectroscopy to investigate the effects of chemical treatment on the exciton emission of 1L-MoS₂. CVD-grown 1L-MoS₂ was treated with bis(trifluoromethane)-sulfonimide (TFSI) or 7,7,8,8-tetracyanoquinodimethane (TCNQ), and nanoscale maps of neutral exciton and trion emission before and after chemical treatment were obtained with 80 nm spatial resolution. A comparison of the local spatial and spectral compositions of neutral excitons and trions suggested that the p-doping effect of TFSI was especially strong around local defects, whereas electron depletion by TCNQ was spatially uniform. The specific reaction of TFSI to defect locations observed in our study provides the clue for the reason that TFSI is notably effective at improving the light emission of 1L-MoS₂.