Gold-Deposited Graphene Nanosheets for Self-Cleaning Graphene Surface-Enhanced Raman Spectroscopy with Superior Charge-Transfer Contribution.

The interaction of graphene with metals initiates charge-transfer interaction-induced chemical enhancements, which critically depend on the doping effect from deposited metallic configurations. In this paper, we have explored the gold nanoparticle-decorated monolayer graphene nanosheets for the large graphene-induced Raman enhancement of adsorbed analytes, indicating the surface-enhanced Raman spectroscopy (SERS) capabilities of metal-doped graphene (G-SERS). Here, the systematically sputtered Au thickness optimization procedure revealed noticeable modifications in the graphene Raman spectra and photoluminescence (PL) background quenching, which indicated favorable charge transfer through n-type doping of chemical vapor deposition-grown graphene nanosheets. The highly consistent, individually distributed morphology of the gold nanoislands over graphene nanosheets depicted a reproducibly uniform G-SERS signal with excellent relative standard deviation values (<5%), resulting in the strongest Raman intensity enhancement factors of ∼10 8 (MB) (methylene blue) and 10 7 (DPA) (2,6-pyridinedicarboxylic acid) composed of the weakest PL background. The combined charge-transfer-induced chemical enhancement and electromagnetic enhancement from individual Au nanoislands result in a lowering of detectability down to 10 -16 M (MB) and 10 -11 M (DPA) concentrations with efficient time-dependent signal stability. Additionally, the GAu demonstrated its effective (∼94.4%) photocatalytic degradation capabilities by decomposing MB dye molecules from a concentration of 1 μM to 2.52 fM within 60 min. Therefore, the prominent charge-transfer contribution through controlled Au decoration over graphene nanosheets provides a potential strategy for fabricating superior SERS sensors and photocatalysts exhibiting adequate signal consistency, stability, and photodegradation efficiency through overcoming the limitations of the traditional sensing platforms.