We present prominent photoresponse of bio-inspired graphene-based phototransistors sensitized with chlorophyll molecules. The hybrid graphene-chlorophyll phototransistors exhibit a high gain of 10^6 electrons per photon and a high responsivity of 10^6 A/W, which can be attributed to the integration of high-mobility graphene and the photosensitive chlorophyll molecules. The charge transfer at interface and the photogating effect in the chlorophyll layer can account for the observed photoresponse of the hybrid devices, which is confirmed by the back-gate-tunable photocurrent as well as the thickness and time dependent studies of the photoresponse. The demonstration of the graphene-chlorophyll phototransistors with high gain envisions a viable method to employ biomaterials for graphene-based optoelectronics.
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