| Summary: | Abstract Great success in 2D van der Waals (vdW) heterostructures based photodetectors is obtained owing to the unique electronic and optoelectronic properties of 2D materials. Performance of photodetectors based 2D vdW heterojunctions at atomic scale is more sensitive to the nanointerface of the heterojunction than conventional bulk heterojunction. Here, a nanoengineered heterostructure for the first‐time demonstration of a nanointerface using an inserted graphene layer between black phosphorus (BP) and InSe which inhibits interlayer recombination and greatly improves photodetection performances is presented. In addition, a transition of the transport characteristics of the device is induced by graphene, from diffusion motion of minority carriers to drift motion of majority carriers. These two reasons together with an internal photoemission effect make the BP/G/InSe‐based photodetector have ultrahigh specific detectivity at room temperature. The results demonstrate that high‐performance vdW heterostructure photodetectors can be achieved through simple structural manipulation of the heterojunction interface on nanoscale.
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