Fast Photoresponse from Hybrid Monolayer MoS2/Organic Photodetector

As a direct‐bandgap transition semiconductor with high carrier mobility, monolayer (ML) transition metal dichalcogenides (TMDCs) have attracted significant attention as a promising class of material for photodetection. It is reported that these layers exhibit a persistent photoconductance (PPC) effect, which is assigned to long‐lasting hole capture by deep traps. Therefore, TMDCs‐based photodetectors show a high photoresponse but also a slow response. Herein, intensity‐modulated photocurrent spectroscopy (IMPS) with steady‐state background illumination is performed to investigate the photoresponse dynamics in a hybrid photodetector based on ML MoS 2 covered with an ultrathin layer of phthalocyanine (H 2 Pc) molecules. The results demonstrate that adding the H 2 Pc layer speeds up the photoresponse of the neat ML‐MoS 2 photodetector by almost two orders of magnitude without deteriorating its responsivity. The origin of these improvements is revealed by applying the Hornbeck–Haynes model to the photocarrier dynamics in the IMPS experiment. It is shown that the improved response speed of the hybrid device arises mostly from a faster detrapping of holes in the presence of the H 2 Pc layer, while the trap densities remain rather unchanged. Meanwhile, the additional absorption of photons in the H 2 Pc layer contributes to photocarrier generation, resulting in an enlarged responsivity of the hybrid device.