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Phys Rev Lett. 2010 Aug 13;105(7):077401. Epub 2010 Aug 10.

Interference between selected dipoles and octupoles in the optical second-harmonic generation from spherical gold nanoparticles.

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  • 1Laboratoire de Spectrométrie Ionique et Moléculaire (LASIM), Université Claude Bernard Lyon 1 - CNRS (UMR 5579), Bâtiment A. Kastler, 43 Boulevard du 11 novembre 1918, 69622 Villleurbanne, France.


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.

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