Optoplasmonic materials comprising both photonic and plasmonic elements are of particular interest for the development of substrates for surface-enhanced Raman spectroscopy (SERS). In this work, a layer of analyte-carrying dielectric nano/microspheres is placed on top of a monolayer of gold nanoparticles to enhance the intensity of the electric (E-) field localization and to enrich the analyte close to the electromagnetic hot spots. Numerical simulations of the hybrid structure confirm an increased and spatially expanded E-field enhancement at the interface. Due to a decreasing filling fraction with increasing size of the dielectric spheres, simulations predict a saturated SERS enhancement for dielectric microspheres with a diameter larger than 4 μm, which is confirmed by experimental SERS measurements. The dielectric microsphere can be functionalized with surface ligands that facilitate the binding of target molecules in solution. The deposition of the analyte-loaded microspheres on the self-assembled gold nanoparticle ensures a high local concentration of analytes in the electromagnetic “hot” surface. The performance of the optoplasmonic SERS approach for detecting methamphetamine in saliva and urine is tested, and the detection of analytes at nanomolar (nM) concentrations is demonstrated.

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