Raman spectroscopy of optical-trapped single particle using bull's eye nanostructure

Surface-enhanced Raman spectroscopy (SERS) has enabled single nanoparticle Raman sensing with abundant applications in analytical chemistry, biomaterials, and environmental monitoring. Genuine single particle Raman sensing requires a cumbersome technique, such as atomic force microscopy (AFM) based tip-enhanced Raman spectroscopy; SERS-based single particle Raman sensing still collects an ensemble signal that samples, in principle, a number of particles. Here, we develop in situ Raman-coupled optical tweezers, based on a hybrid nanostructure consisting of a single bowtie aperture surrounded by bull's eye rings, to trap and excite a rhodamine-6G-dye-doped polystyrene sphere. We simulated a platform to ensure sufficient enhancement capability for both optical trapping and SERS of a single nanoparticle. Experiments with well-designed controls clearly attribute the Raman signal origin to a single 15-nm particle trapped at the center of a nanohole, and they also clarified the trapping and Raman enhancement role of the bull's eye rings. We claim Raman sensing of a smallest optically trapped particle.