Symmetry selective third harmonic generation from plasmonic metacrystals

Abstract: Nonlinear processes are often governed by selection rules imposed by the symmetries of the molecular configurations. The most well-known examples include the role of mirror symmetry breaking for the generation of even harmonics, and the selection rule related to the rotation symmetry in harmonic generation for fundamental beams with circular polarizations. While the role of mirror symmetry breaking in second harmonic generation has been extensively studied in plasmonic systems, the investigation on selection rules pertaining to circular polarization states of harmonic generation has been limited to crystals, i.e. symmetries at the atomic level. Here we demonstrate the rotational symmetry dependent third harmonic generation from nonlinear plasmonic metacrystals. We show that the selection rule can be imposed by the rotational symmetry of meta-crystals embedded into an isotropic organic nonlinear thin film. The results presented here may open new avenues for designing symmetry-dependent nonlinear optical responses with tailored plasmonic nanostructures.