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Surface enhanced Raman scattering (SERS) is optically sensitive andchemically specific to detect single molecule spectroscopic signatures.Facilitating this capability in optically-trapped nanoparticles at low laserpower remains a significant challenge. In this letter, we show single moleculeSERS signatures in reversible assemblies of trapped plasmonic nanoparticlesusing a single laser excitation (633 nm). Importantly, this trap is facilitatedby the thermoplasmonic field of a single gold nanoparticle dropcasted on aglass surface. We employ bi-analyte SERS technique to ascertain the singlemolecule statistical signatures, and identify the critical parameters of thethermoplasmonic tweezer that provide this sensitivity. Furthermore, we show theutility of this low power ($\approx$0.1 mW/$\mu$m^2) tweezer platform to trapsingle gold nanoparticle and transport assembly of nanoparticles. Given thatour configuration is based on a dropcasted gold nanoparticle, we envisage itsutility to create reconfigurable plasmonic metafluids in physiological andcatalytic environments, and can be potentially adapted as an in-vivo plasmonictweezer.

Single Molecule SERS in a Single Gold Nanoparticle-driven Thermoplasmonic Tweezer