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Single-molecule surface enhanced Raman scattering (SM-SERS) is one of thevital applications of plasmonic nanoparticles. The SM-SERS sensitivitycritically depends on plasmonic hot-spots created at the vicinity of suchnanoparticles. In conventional fluid-phase SM-SERS experiments, plasmonichot-spots are facilitated by chemical aggregation of nanoparticles. Suchaggregation is usually irreversible, and hence, nanoparticles cannot bere-dispersed in the fluid for further use. Here, we show how to combine SM-SERSwith plasmon-polariton assisted, reversible assembly of plasmonic nanoparticlesat an unstructured metal-fluid interface. One of the unique features of ourmethod is that we use a single evanescent-wave optical excitation fornanoparticle-assembly, manipulation and SM-SERS measurements. Furthermore, byutilizing dual excitation of plasmons at metal-fluid interface, we createinteracting assemblies of metal nanoparticles, which may be further harnessedin dynamic lithography of dispersed nanostructures. Our work will haveimplications in realizing optically addressable, plasmofluidic, single-moleculedetection platforms.

Plasmofluidic Single-Molecule Surface Enhanced Raman Scattering from Dynamic Assembly of Plasmonic Nanoparticles