Recombination Kinetics and Effects of Superacid Treatment in Sulfur- and Selenium-Based Transition Metal Dichalcogenides

Optoelectronic devices based on two-dimensional (2D) materials have shown tremendous promise over the past few years; however, there are still numerous challenges that need to be overcome to enable their application in devices. These include improving their poor photoluminescence (PL) quantum yield (QY) as well as better understanding of exciton-based recombination kinetics. Recently, we developed a chemical treatment technique using an organic superacid, bis(trifluoromethane)sulfonimide (TFSI), which was shown to improve the quantum yield in MoS₂ from less than 1% to over 95%. Here, we perform detailed steady-state and transient optical characterization on some of the most heavily studied direct bandgap 2D materials, specifically WS₂, MoS₂, WSe₂, and MoSe₂, over a large pump dynamic range to study the recombination mechanisms present in these materials. We then explore the effects of TFSI treatment on the PL QY and recombination kinetics for each case. Our results suggest that sulfur-based 2D materials are amenable to repair/passivation by TFSI, while the mechanism is thus far ineffective on selenium based systems. We also show that biexcitonic recombination is the dominant nonradiative pathway in these materials and that the kinetics for TFSI treated MoS₂ and WS₂ can be described using a simple two parameter model.