Toy model of harmonic and sum frequency generation in 2D nanostructures.

Optical nonlinearities of matter are often associated with the response of individual atoms. Here, using a toy oscillator model, we show that in the confined geometry of a two-dimensional dielectric nanoparticle a collective nonlinear response of the atomic array can arise from the Coulomb interactions of the bound optical electrons, even if the individual atoms exhibit no nonlinearity. We determine the multipole contributions to the nonlinear response of nanoparticles and demonstrate that the odd order and even order nonlinear electric dipole moments scale with the area and perimeter of the nanoparticle, respectively.