Asymmetric contact pairs with different work functions provide an efficient method to extract photogenerated carriers in optoelectrical devices. Specifically, vertical optoelectrical devices based on two-dimensional (2D) materials utilize graphene layers as the bottom and top contacts. Whereas an additional terminal is required for electrostatic doping in either top or bottom graphene to enlarge the built-in electric field. Herein, we present an enhanced photovoltaic response in a vertical WSe2 photodetector utilizing asymmetric 2D contacts. A graphite layer and a degenerate SnSe2 are used as the top and bottom contacts, respectively, with a significant difference in their work functions. By establishing a large built-in electric field across the vertical WSe2 layer, a strong photovoltaic effect is achieved, resulting in an open-circuit voltage of 0.37 V and a short-circuit current of 0.42 μA under 532 nm illumination. The device shows high-performance photodetection characteristics, with a responsivity of 32.04 A W−1, external quantum efficiency of 7475%, and specific detectivity of 3.61 × 1012 Jones. Furthermore, the device can generate a maximum output electrical power of 70.9 nW, enabling a high-power conversion efficiency of 3.5%.
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