We have measured ultrafast charge carrier dynamics in monolayers and trilayers of the transition metal dichalcogenides MoS₂ and WSe₂ using a combination of time-resolved photoluminescence and terahertz spectroscopy. We recorded a photoconductivity and photoluminescence response time of just 350 fs from CVD-grown monolayer MoS₂, and 1 ps from trilayer MoS₂ and monolayer WSe₂. Our results indicate the potential of these materials as high-speed optoelectronic materials.

Significance: We use transient spectroscopy to investigate the mechanism of singlet exciton fission, a quantum mechanical phenomenon in some organic molecules in which a spin-singlet excited state can split into two spin-triplet states. This process may be harnessed to boost solar cell efficiencies, but the underlying mechanism remains poorly understood. Central to most models is a triplet pair state, consisting of two triplets entangled into an overall spin-singlet configuration, but it has never before been optically detected. In a solution-based system, we detect a state with simultaneous singlet and triplet exciton character that dissociates to form triplet excitons in 120% yield. We consider that this intermediate constitutes a triplet pair state, and its observation allows important insight into the nature of triplet exciton coupling.