Delocalization of Nonlinear Optical Responses in Plasmonic Nanoantennas

Remote excitation and emission of two-photon luminescence and second-harmonic generation are observed in micrometer long gold rod optical antennas upon local illumination with a tightly focused near-infrared femtosecond laser beam. We show that these nonlinear radiations are emitted from the entire antenna and the measured far-field angular patterns bear the information regarding the nature and origins of the respective nonlinear processes. We demonstrate that the nonlinear responses are locally induced by a propagating surface plasmon at the excitation frequency, enabling thereby a polariton-mediated spatial tailoring and design of coherent and incoherent nonlinear responses.