Surface second-harmonic generation from coupled spherical plasmonic nanoparticles: Eigenmode analysis and symmetry properties

The surface second-harmonic generation from interacting spherical plasmonic nanoparticles building different clusters (symmetric and asymmetric dimers, trimers) is theoretically investigated. The plasmonic eigenmodes of the nanoparticle clusters are first determined using an ab initio approach based on the Green's functions method. This method provides the properties, such as the resonant wavelengths, of the modes sustained by a given cluster. The fundamental and second-harmonic responses of the corresponding clusters are then calculated using a surface integral method. The symmetry of both the linear and nonlinear responses is investigated, as well as their relationship. It is shown that the second-harmonic generation can be significantly enhanced when the fundamental field is such that its second harmonic matches modes with suitable symmetry. The role played by the nanogaps in second-harmonic generation is also underlined. The results presented in this article demonstrate that the properties of the second-harmonic generation from coupled metallic nanoparticles cannot be fully predicted from their linear response only, while, on the other hand, a detailed knowledge of the underlying modal structure can be used to optimize the generation of the second harmonic.