Multipolar analysis of second-harmonic radiation from gold nanoparticles

We present a multipolar tensor analysis of second-harmonic radiation from arrays of noncentrosymmetric L-shaped gold nanoparticles. Our approach is based on the fundamental differences in the radiative properties of electric dipoles and higher multipoles, which give rise to differences in the nonlinear response tensors for the reflected and transmitted second-harmonic signals. The results are analyzed by dividing the tensors into symmetric (dipolar) and antisymmetric (higher multipolar) parts between the two directions. The nonlinear response is found to be dominated by a tensor component, not resolved earlier [Phys. Rev. Lett. 98, 167403 (2007)], which is associated with chiral symmetry breaking of the sample and which also contains a strong multipolar contribution. The results are explained by a phenomenological model where asymmetrically-distributed defects on opposite sides of the particles give rise to dipolar and quadrupolar second-harmonic emission.