We demonstrate that second-harmonic generation (SHG) from arrays of non-centrosymmetric T-shaped gold nanodimers with a nanogap arises from asymmetry in the local fundamental field distribution and is not related strictly to nanogap size. Calculations show that the local field contains orthogonal polarization components not present in the exciting field, which yield the dominant SHG response. The strongest SHG responses occur through the local surface susceptibility of the particles for a fundamental field distributed asymmetrically at the particle perimeters. Weak responses result from more symmetric distributions despite high field enhancement in the nanogap. Nearly constant field enhancement persists for relatively large nanogap sizes.

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.

We prepare arrays of gold nanoparticles that include both noncentrosymmetric particles with a second-order nonlinear optical response (active particles) and centrosymmetric particles with no second-order response (passive particles). The plasmon resonances of the active and passive particles are at distinct wavelengths, yet the passive particles modify the electromagnetic modes of the structure in such a way that second-harmonic generation from the active particles is enhanced. Our results provide a completely new concept for optimizing the nonlinear responses of metamaterials.

We demonstrate that optical second-harmonic generation (SHG) from arrays of noncentrosymmetric gold nanoparticles depends essentially on particle geometry. We prepare nanoparticles with different geometrical shapes (L and T) but similar wavelengths for the polarization-dependent plasmon resonances. In contrast to recent interpretations emphasizing resonances at the fundamental frequency, the T shape leads to stronger SHG when only one, instead of both, polarization component of the fundamental field is resonant. This is explained by the character of plasmon oscillations supported by the two shapes. Our numerical simulations for both linear and second-order responses display unprecedented agreement with measurements.

Second-harmonic generation from T-shaped gold nanodimers with nanogaps has different efficiencies for left- and right-hand circularly polarized fundamental light. The difference arises from the chiral symmetry breaking of the dimers due to nonorthogonal mutual orientations of the horizontal and vertical bars of the T shape and depends on the gap size. Unexpectedly, the smallest gap with presumably the strongest coupling gives rise to only a small difference. All results can be explained by considering the distribution of the polarized local field in the structure.