Tunable Nanoislands Decorated Tapered Optical Fibers Reveal Concurrent Contributions in Through-Fiber SERS Detection

Creating plasmonic nanoparticles on a tapered optical fiber (TF) tip enables a remote surface-enhanced Raman scattering (SERS) sensing probe, ideal for challenging sampling scenarios like biological tissues, site-specific cells, on-site environmental monitoring, and deep brain structures. However, nanoparticle patterns fabricated from current bottom-up methods are mostly random, making geometry control difficult. Uneven statistical distribution, clustering, and multilayer deposition introduce uncertainty in correlating device performance with morphology. Ultimately, this limits the design of the best-performance remote SERS sensing probe. Here we employ a tunable solid-state dewetting method to create densely packed monolayer Au nanoislands with varied geometric parameters in direct contact with the silica TF surface. These patterns exhibit analyzable nanoparticle sizes, densities, and uniform distribution across the entire taper surface, enabling a systematic investigation of particle size, density, and analyte effects on the SERS performance of the through-fiber detection system. The study is focused on the SERS response of a widely employed benchmark molecule, rhodamine 6G (R6G), and serotonin, a highly relevant neurotransmitter for the neuroscience field. The numerical simulations and limit of detection (LOD) experiments on R6G show that the increase of the total near-field enhancement volume promotes the SERS sensitivity of the probe. However, we observed a different behavior for serotonin linked to its interaction with the nanoparticle's surface. The obtained LOD is as low as 10^-7 M, a value not achieved so far in a through-fiber detection scheme. Therefore, our work offers a strategy to design nanoparticle-based remote SERS sensing probes and provides new clues to discover and understand intricate plasmonic-driven chemical reactions.