▎ 摘　　要

Biomolecule/graphene van der Waals heterojunction provides a generic platform for designing high-performance, flexible, and scalable optoelectronics. A key challenge is, in controllable attachment, the biomolecules to form a desired interfacial electronic structure for a high-efficiency optoelectronic process of photoabsorption, exciton dissociation into photocarriers, carrier transfer, and transport. Here, it is shown that a polarity-controlled attachment of the Cytochrome c (Cyt c) biomolecules can be achieved on the channel of graphene field effect transistors (GFET). High-efficiency charge transfer across the formed Cyt c/graphene interface is demonstrated when Cyt c attaches with positively charged side to GFET as predicted by molecular dynamics simulation and confirmed experimentally. This Cyt c/GFET van der Waals heterojunction nanohybrid photodetector exhibits a spectral photoresponsivity resembling the absorption spectrum of the Cyt c, confirming the role of Cty c as the photosensitizer in the device. The high visible photoresponsivity up to 7.57 x 10(4) A W-1 can be attributed to the high photoconductive gain in exceeding 10(5) facilitated by the high carrier mobility in graphene. This result therefore demonstrates a viable approach in synthesis of the biomolecule/graphene van der Waals heterojunction optoelectronics using polarity-controlled biomolecule attachment, which can be expanded for on-chip printing of high-performance molecular optoelectronics.