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In this study,we combined time-resolved terahertz spectroscopy along withtransient absorption spectroscopy to revisit the interlayer non-equilibriumcarrier dynamics in largely lateral size Gr/MoS2 heterostructure fabricatedwith chemical vapor deposition method. Our experimental results reveal that,with photon-energy below the A-exciton of MoS2 monolayer, hot electronstransfer from graphene to MoS2 takes place in time scale of less than 0.5 ps,resulting in ultrafast formation of interfacial exciton in the heterostructure,subsequently, recombination relaxation of the interfacial exciton occurs intime scale of ~18 ps. A new model considering carrier heating and photogatingeffect in graphene is proposed to estimate the amount of carrier transfer inthe heterostructure, which shows a good agreement with experimental result.Moreover, when the photon-energy is on-resonance with the A-exciton of MoS2,photogenerated holes in MoS2 are transferred to graphene layer within 0.5 ps,leading to the formation of interfacial exciton, the subsequentphotoconductivity (PC) relaxation of graphene and bleaching recovery ofA-exciton in MoS2 take place around ~10 ps time scale, ascribing to theinterfacial exciton recombination. The faster recombination time of interfacialexciton with on-resonance excitation could come from the reduced interfacebarrier caused by bandgap renormalization effect. Our study provides deepinsight into the understanding of interfacial charge transfer as well as therelaxation dynamics in graphene-based heterostructures, which are promising forthe applications of graphene-based optoelectronic devices.

Observation of Ultrafast Interfacial Exciton Formation and Recombination in Graphene/MoS2 Heterostructure