Bridging the van der Waals Interface for Advanced Optoelectronic Devices

Abstract Van der Waals (vdW) heterostructures exhibit excellent optoelectronic properties and novel functionalities. However, their applicability is impeded due to the common issue of the tunneling barrier, which arises from the vdW gap; this significantly increases the injection resistance of the photoexcited carriers. Herein, a generic strategy is demonstrated to eliminate the vdW gap in a broad class of heterostructures. It is observed that the vdW gap in the interface is bridged via strong orbital hybridization between the interface dangling bonds of nonlayered chalcogenide semiconductors and the artificially induced vacancies of transition metal chalcogenides (TMDCs). The photoresponse times of bridged PbS/ReS 2 , PbS/MoSe 2 , and PbS/MoS 2 are ≈30, 51, and 43 µs, respectively. The photon‐triggered on/off ratio of the bridged PbS/MoS 2 , ZnSe/MoS 2 , and ZnTe/MoS 2 heterostructures exceed 10 6 , 10 5 , and 10 5 , respectively. These are several orders of magnitude higher than common vdW heterostructures. The findings obtained in this study present a versatile strategy for overcoming the performance limitations of vdW heterostructures.