Defect-Rich Monolayer MoS2 as a Universally Enhanced Substrate for Surface-Enhanced Raman Scattering

Abstract

Monolayer 2H-MoS2 has been widely noticed as a typical transition metal dichalcogenides (TMDC) for surface-enhanced Raman scattering (SERS). However, monolayer MoS2 is limited to a narrow range of applications due to poor detection sensitivity caused by the combination of a lower density of states (DOS) near the Fermi energy level as well as a rich fluorescence background. Here, surfaced S and Mo atomic defects are fabricated on a monolayer MoS2 with a perfect lattice. Defects exhibit metallic properties. The presence of defects enhances the interaction between MoS2 and the detection molecule, and it increases the probability of photoinduced charge transfer (PICT), resulting in a significant improvement of Raman enhancement. Defect-containing monolayer MoS2 enables the fluorescence signal of many dyes to be effectively burst, making the SERS spectrum clearer and making the limits of detection (LODs) below 10−8 M. In conclusion, metallic defect-containing monolayer MoS2 becomes a promising and versatile substrate capable of detecting a wide range of dye molecules due to its abundant DOS and effective PICT resonance. In addition, the synergistic effect of surface defects and of the MoS2 main body presents a new perspective for plasma-free SERS based on the chemical mechanism (CM), which provides promising theoretical support for other TMDC studies.