Self-powered photodetectors hold great promise for addressing power-related challenges in the “Internet of Things (IoT)” era. However, the self-powered performances of a metal-semiconductor-metal (MSM) structure photodetector are inherently limited due to the presence of the symmetric Schottky contacts, leading to canceling photocurrents in opposite directions, while constructing an asymmetric MSM structure demands complicated design or sustained external fields. Herein, we propose a novel contact engineering strategy based on localized femtosecond (fs) laser irradiation, achieving an asymmetric band structure in an MSM-structure photodetector with pristine symmetric Schottky contacts. As a result, a MoS2 photodetector that exhibits exceptional photoresponse and self-powered performances is successfully fabricated. The device type transitions from a photoconductor to a photodiode, exhibiting a significant improvement in the rectification ratio from 1 to > 104. A comprehensive study on fs laser-based contact engineering is conducted by investigating atom diffusion, element variation, and Schottky barrier height variation. Notably, the photodetector demonstrates an exceptional zero-bias responsivity of 1.72 A/W, with a short circuit current of 37.2 nA and maximum output electric power of 1.67 nW. Our work provides a new strategy for modifying the energy band structure and facilitates the fabrication of high-performance self-powered photodetectors.
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