Switchable Photoresponse Mechanisms Implemented in Single van der Waals Semiconductor/Metal Heterostructure

van der Waals (vdW) heterostructures based on two-dimensional (2D) semiconducting materials have been extensively studied for functional applications, and most of the reported devices work with sole mechanism. The emerging metallic 2D materials provide us new options for building functional vdW heterostructures via rational band engineering design. Here, we investigate the vdW semiconductor/metal heterostructure built with 2D semiconducting InSe and metallic 1T-phase NbTe₂, whose electron affinity χ_InSe and work function Φ_NbTe2 almost exactly align. Electrical characterization verifies exceptional diode-like rectification ratio of >10³ for the InSe/NbTe₂ heterostructure device. Further photocurrent mappings reveal the switchable photoresponse mechanisms of this heterostructure or, in other words, the alternative roles that metallic NbTe₂ plays. Specifically, this heterostructure device works in a photovoltaic manner under reverse bias, whereas it turns to phototransistor with InSe channel and NbTe₂ electrode under high forward bias. The switchable photoresponse mechanisms originate from the band alignment at the interface, where the band bending could be readily adjusted by the bias voltage. In addition, a conceptual optoelectronic logic gate is proposed based on the exclusive working mechanisms. Finally, the photodetection performance of this heterostructure is represented by an ultrahigh responsivity of ∼84 A/W to 532 nm laser. Our results demonstrate the valuable application of 2D metals in functional devices, as well as the potential of implementing photovoltaic device and phototransistor with single vdW heterostructure.