Ultrafast Electron Transfer with Long-Lived Charge Separation and Spin Polarization in WSe<sub>2</sub>/C<sub>60</sub> Heterojunction
Chang Zhao, Weijian Tao, Zeng Chen, Hongzhi Zhou, Chi Zhang, Junyi Lin, Haiming Zhu
Abstract
The strong excitonic effect in monolayer transition-metal dichalcogenides (TMDs) endows them with intriguing optoelectronic properties but also short-lived population and valley polarization. Exciton dissociation by interfacial charge transfer has been shown as an effective approach to prolonging excited-state lifetimes. Herein, by ultrafast spectroscopy and building-block molecule C60, we investigated exciton and valley polarization dynamics in the prototypical WSe2/C60 inorganic–organic hybrid. We show that excitons in WSe2 can be dissociated through ultrafast (∼1 ps) electron transfer to C60, with nanosecond charge separation due to thermally activated electron diffusion in C60 film. Because of suppressed electron–hole exchange interaction after electron transfer, hole in WSe2 exhibits a spin/valley polarization lifetime of ∼60 ps at room temperature, more than 2 orders of magnitude longer than that in WSe2 monolayer. This study suggests exciton dissociation as a general approach to suppress electron–hole interaction and prolong the charge/spin/valley lifetime in TMDs.