Direct Observation of Charge Injection of Graphene in the Graphene/WSe₂ Heterostructure by Optical-Pump Terahertz-Probe Spectroscopy

Charge transfer across the interface and interlayer coupling in the graphene van der Waals heterostructure, which is constructed by graphene and semiconducting transition metal dichalcogenides (TMDCs), is critical for their electronic and optoelectronic applications. Photo-induced charge injection from TMDC to graphene has been studied in several heterostructure photodetectors. However, the response time significantly varies among different reports, ranging from microseconds to milliseconds. In this work, using a graphene/WSe2 heterostructure as an example, we directly observe the carrier density change in graphene by time-resolved optical-pump terahertz (THz)-probe spectroscopy and show the ultrafast picosecond photoresponse of graphene. In the absence of photoexcitation, THz time-domain spectroscopic measurements show that WSe2 can transfer holes to graphene and pull down the Fermi level of graphene. After excitation by the ultrafast laser pulse, the transient THz response shows a rapid (∼0.35 ps) increase in the graphene conductivity mainly due to the hole injection from WSe2 into graphene. Unlike previous reports on band bend as the guidance mechanism for charge transfer, our results show that the relevant mechanism is the band offset across the atomically sharp interface.