Metamaterials with tailored nonlinear optical response.

We demonstrate that the second-order nonlinear optical response of noncentrosymmetric metal nanoparticles (metamolecules) can be efficiently controlled by their mutual ordering in an array. Two samples with minor change in ordering have nonlinear responses differing by a factor of up to 50. The results arise from polarization-dependent plasmonic resonances modified by long-range coupling associated with metamolecular ordering. The approach opens new ways for tailoring the nonlinear responses of metamaterials and their tensorial properties.