Low-temperature photocarrier dynamics in single-layer MoS2 flakes

The dichalcogenide MoS2, which is an indirect-gap semiconductor in its bulk form, was recently shown to become an efficient emitter of photoluminescence as it is thinned to a single layer, indicating a transition to a direct-gap semiconductor due to confinement effects. With its layered structure of weakly coupled, covalently bonded two-dimensional sheets, it can be prepared, just as graphene, using mechanical exfoliation techniques. Here, we present temperature-dependent and time-resolved photoluminescence (PL) studies of single-layer MoS2 flakes. Some of the flakes are covered with oxide layers prepared by atomic layer deposition (ALD). At low temperatures, we clearly see two PL peaks in the as-prepared flakes without oxide layers, which we may assign to bound and free exciton transitions. The lower-energy, bound exciton PL peak is absent in the oxide-covered flakes. In time-resolved PL measurements, we observe very fast photocarrier recombination on the few-ps timescale at low temperatures, with increasing photocarrier lifetimes at higher temperatures due to exciton-phonon scattering.