Unraveling the Raman Enhancement Mechanism on 1T′‐Phase ReS 2 Nanosheets

2D transition metal dichalcogenides materials are explored as potential surface‐enhanced Raman spectroscopy substrates. Herein, a systematic study of the Raman enhancement mechanism on distorted 1T (1T′) rhenium disulfide (ReS 2 ) nanosheets is demonstrated. Combined Raman and photoluminescence studies with the introduction of an Al 2 O 3 dielectric layer unambiguously reveal that Raman enhancement on ReS 2 materials is from a charge transfer process rather than from an energy transfer process, and Raman enhancement is inversely proportional while the photoluminescence quenching effect is proportional to the layer number (thickness) of ReS 2 nanosheets. On monolayer ReS 2 film, a strong resonance‐enhanced Raman scattering effect dependent on the laser excitation energy is detected, and a detection limit as low as 10 −9 m can be reached from the studied dye molecules such as rhodamine 6G and methylene blue. Such a high enhancement factor achieved through enhanced charge interaction between target molecule and substrate suggests that with careful consideration of the layer‐number‐dependent feature and excitation‐energy‐related resonance effect, ReS 2 is a promising Raman enhancement platform for sensing applications.