Controlling Photocarrier Lifetime in Graphene for Enhanced Photocurrent Generation via Cascade Hot Electron Transfer

Because of its broad absorption and high carrier mobility, graphene has been regarded as a promising photoactive material for optoelectronics. However, its ultrashort photoexcited carrier lifetime greatly restricts the device performance. Herein, we show that by constructing a graphene/WS₂/MoS₂ vertical heterostructure with a cascade electron-transfer pathway, the hot electrons in graphene under low-energy photoexcitation can efficiently transfer through WS₂ to MoS₂ in 180 fs, thus effectively photogating the graphene layer. Because of the spatial separation and energy barrier imposed by the WS₂ intermediate layer which retards back electron transfer, the photocarrier lifetime in graphene is significantly prolonged to ∼382.7 ps, more than 2 orders of magnitude longer than in isolated graphene and graphene/WS₂ binary heterostructure. The prolonged photocarrier lifetime in graphene leads to dramatically enhanced photocurrent generation and photoresponsivity. This study offers an exciting approach to control photocarrier lifetime in graphene for hot carrier devices with simultaneous broadband and high responsivity.