Controllable Nanoparticle Aggregation through a Superhydrophobic Laser-Induced Graphene Dynamic System for Surface-Enhanced Raman Scattering Detection

Surface-enhanced Raman scattering (SERS) is widely used for low-concentration molecular detection; however, challenges related to detection uniformity and repeatability are bottlenecks for practical application, especially as regards ultrasensitive detection. Here, through the coupling of bionics and fluid mechanics, a lotus-leaf effect and rose-petal effect (LLE-RPE)-integrated superhydrophobic chip is facilely developed using laser-induced graphene (LIG) fabricated on a polyimide film. Dense and uniform aggregation of gold nanoparticles (AuNPs) in droplets is realized through a constant contact angle (CCA) evaporation mode in the dynamic enrichment process, facilitating reliable ultrasensitive detection. The detection chip consists of two components: an LLE zone containing an ethanol-treated LIG superhydrophobic surface with a low-adhesive property, which functions as an AuNP-controllable aggregation zone, and an RPE zone containing an as-fabricated LIG superhydrophobic surface with water-solution pinning ability, which functions as a droplet solvent evaporation and a AuNP blending zone. AuNPs realize uniform aggregation during rolling on the LLE zone, and then get immobilized on the RPE zone to complete evaporation of the solvent, followed by Raman detection. Here, based on dense and uniform AuNP aggregation, the detection system achieves high-efficiency (242 s/18 μL) and ultralow-concentration (10-17 M) detection of a target analyte (rhodamine 6G). The proposed system constitutes a simple approach toward high-performance detection for chemical analysis, environmental monitoring, biological analysis, and medical diagnosis.