Many potential applications of monolayer transition metal dichalcogenides (TMDs) require both high photoluminescence (PL) yield and high electrical mobilities. However, the PL yield of as prepared TMD monolayers is low and believed to be limited by defect sites and uncontrolled doping. This has led to a large effort to develop chemical passivation methods to improve PL and mobilities. The most successful of these treatments is based on the nonoxidizing organic “superacid” bis(trifluoromethane)sulfonimide (TFSI) which has been shown to yield bright monolayers of molybdenum disulfide (MoS2) and tungsten disulfide (WS2) but with trap-limited PL dynamics and no significant improvements in field effect mobilities. Here, using steady-state and time-resolved PL microscopy we demonstrate that treatment of WS2 monolayers with oleic acid (OA) can greatly enhance the PL yield, resulting in bright neutral exciton emission comparable to TFSI treated monolayers. At high excitation densities, the OA treatment allows for bright trion emission, which has not been demonstrated with previous chemical treatments. We show that unlike the TFSI treatment, the OA yields PL dynamics that are largely trap free. In addition, field effect transistors show an increase in mobilities with the OA treatment. These results suggest that OA serves to passivate defect sites in the WS2 monolayers in a manner akin to the passivation of colloidal quantum dots with OA ligands. Our results open up a new pathway to passivate and tune defects in monolayer TMDs using simple “wet” chemistry techniques, allowing for trap-free electronic properties and bright neutral exciton and trion emission.
While there have been numerous reports of long-range polariton transport at room-temperature in organic cavities, the spatiotemporal evolution of the propagation is scarcely reported, particularly in the initial coherent sub-ps regime, where photon and exciton wavefunctions are inextricably mixed. Hence the detailed process of coherent organic exciton-polariton transport and, in particular, the role of dark states has remained poorly understood. Here, femtosecond transient absorption microscopy is used to directly image coherent polariton motion in microcavities of varying quality factor. The transport is found to be well-described by a model of band-like propagation of an initially Gaussian distribution of exciton-polaritons in real space. The velocity of the polaritons reaches values of ≈ 0.65 × 10 6 m s −1 , substantially lower than expected from the polariton dispersion. Further, it is found that the velocity is proportional to the quality factor of the microcavity. This unexpected link between the quality-factor and polariton velocity is suggested to be a result of varying admixing between delocalized dark and polariton states.
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