Photoresponse-Bias Modulation of a High-Performance MoS2 Photodetector with a Unique Vertically Stacked 2H-MoS2/1T@2H-MoS2 Structure.

Monolayer 2H-phase MoS2-based photodetectors exhibit high photon absorption but suffer from low photoresponse, which severely limits their applications in optoelectronic fields. The metallic 1T phase of MoS2, while transporting carriers faster, shows negligible response to visible light, which limits its usage in photodetectors. Herein, we propose an ultrafast-response MoS2-based photodetector having a channel that consists of a 2H-MoS2 sensitizing monolayer on top of 1T@2H-MoS2. The 1T@2H-MoS2 layer has a thickness of several nanometers and is a mixture of metallic 1T-MoS2 and semiconducting 2H-MoS2, imparting metal-like properties to the photodetector. Compared with the monolayer 2H-MoS2 photodetector, we observed a drastic increase in the photoresponse of the 2H-MoS2/1T@2H-MoS2 vertically stacked photodetector to a value of 1917 A W-1. Owing to the presence of metallic 1T-MoS2 within the metal-like 1T@2H-MoS2, the performance of the 2H-MoS2/1T@2H-MoS2 vertically stacked photodetector is voltage bias-modulated with an external quantum efficiency (EQE) of up to 448,384% and a specific detectivity of up to ∼1011 Jones. The higher carrier density and higher mobility of the 1T@2H-MoS2 layer explain the better bias-modulated performance. In addition, the interface between 2H-MoS2 and 1T@2H-MoS2 ensures fewer dangling bonds and reduced lattice mismatching. Thus, this study presents an exclusive vertically stacked MoS2-based photodetector that lays the foundation for the development of photodetectors exhibiting higher photoresponse.