Engineering Photonic-Plasmonic Coupling in Metal Nanoparticle Necklaces

In this paper, by combining three-dimensional finite-difference time-domain simulations, dark-field scattering analysis, and surface-enhanced Raman spectroscopy (SERS) we systematically investigate the light-scattering and field localization properties of circular loops of closely spaced gold nanoparticles, or nanoplasmonic necklaces, fabricated by electron-beam lithography on quartz substrates. In particular, we Show that nanoplasmonic necklaces support two hybridized dipolar scattering resonances with polarization-controlled subwavelength localized fields (i.e., electromagnetic hot-spots), whose intensities are optimized by varying the necklace particle diameter and the particle number. Moreover, we show that strong field intensity enhancement is obtained for the particular necklace diameters where loop-localized photonic resonances efficiently couple to the broadband plasmonic modes, enabling a simple design strategy for the optimization of electromagnetic near-fields. Following the proposed approach, we design nanoplasmonic necklaces supporting stronger field intensity enhancement than traditional nanoparticle monomer and dimer arrays. Finally, by performing SERS experiments on nanoplasmonic necklaces coated with a pMA molecular monolayer, we validate the optimization of their near-field properties and demonstrate their potential for plasmon-enhanced spectroscopy and sensing.