Plasmonic systems are known for their distinct nonlinear optical properties when compared to purely dielectric materials. Although it is well accepted that the enhanced nonlinear processes in plasmonic-dielectric compounds are related to the excitation of localized plasmon resonances, their exact origin is concealed by the local field enhancement in the surrounding material and the nonlinearity in the metal. Here, we show that the origin of third-harmonic generation in hybrid plasmonic-dielectric compounds can be unambiguously identified from the shape of the nonlinear spectrum.

• Received 12 November 2010

DOI:https://doi.org/10.1103/PhysRevLett.106.133901