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Doping of Monolayer Transition-Metal Dichalcogenides via Physisorption of Aromatic Solvent Molecules.

Two-dimensional (2D) transition-metal dichalcogenides (TMDs) recently emerged as novel materials displaying a wide variety of physicochemical properties that render them unique scaffolds for high-performance (opto)electronics. The controlled physisorption of molecules on the TMD surface is a viable approach for tuning their optical and electronic properties. Solvents, made of small aromatic molecules, are frequently employed for the cleaning of the 2D materials or as a "dispersant" for their chemical functionalization with larger (macro)molecules, without considering their potential key effect in locally modifying the characteristics of 2D materials. In this work, we demonstrate how the electronic and optical properties of a mechanically exfoliated monolayer of MoS2 and WSe2 are modified when physically interacting with small aromatic molecules of common solvents. Low-temperature photoluminescence (PL) spectra recorded at 78 K revealed that physisorbed benzene derivatives could modulate the charge carrier density in monolayer TMDs, hence affecting the switching between a neutral exciton and trion (charged exciton). By combining experimental evidence with density functional theory calculations, we confirm that charge-transfer doping on TMDs depends not only on the difference in chemical potential between molecules and 2D materials but also on the thermodynamic stability of physisorption. Our results provide unambiguous evidences of the great potential of optical and electrical tuning of monolayer MoS2 and WSe2 by physisorption of small aromatic solvent molecules, which is highly relevant for both fundamental studies and device application purposes.