Highly Stable Near-Unity Photoluminescence Yield in Monolayer MoS₂ by Fluoropolymer Encapsulation and Superacid Treatment

Recently, there has been considerable research interest in two-dimensional (2D) transition-metal dichalcogenides (TMDCs) for future optoelectronic applications. It has been shown that surface passivation with the organic nonoxidizing superacid bis(trifluoromethane)sulfonamide (TFSI) produces MoS₂ and WS₂ monolayers whose recombination is at the radiative limit, with a photoluminescence (PL) quantum yield (QY) of ∼100%. While the surface passivation persists under ambient conditions, exposure to conditions such as water, solvents, and low pressure found in typical semiconductor processing degrades the PL QY. Here, an encapsulation/passivation approach is demonstrated that yields near-unity PL QY in MoS₂ and WS₂ monolayers which are highly stable against postprocessing. The approach consists of two simple steps: encapsulation of the monolayers with an amorphous fluoropolymer and a subsequent TFSI treatment. The TFSI molecules are able to diffuse through the encapsulation layer and passivate the defect states of the monolayers. Additionally, we demonstrate that the encapsulation layer can be patterned by lithography and is compatible with subsequent fabrication processes. Therefore, our work presents a feasible route for future fabrication of highly efficient optoelectronic devices based on TMDCs.