Optical second-harmonic generation from gold nanoparticles is investigated both experimentally and theoretically. The contribution of octupoles is reported for the first time in the second-harmonic emission pattern, by using an harmonic polarization in the scattering plane. The experimental results presented here for particle sizes up to 100 nm are in excellent agreement with finite element method simulations involving the normal surface term only in the nonlinear polarization source. In addition, analytical calculations based on nonlinear Mie scattering theory clearly evidence the constructive and destructive interferences occurring between the dipolar and octupolar responses selected with this polarization configuration.

• Received 21 April 2010

DOI:https://doi.org/10.1103/PhysRevLett.105.077401