Nonlinear optical response from single spheres coated by a nonlinear monolayer

We detected the second-order nonlinear response from single isolated spheres comprised from a centrosymmetric material but covered by a layer of a material with strong second-order nonlinear properties and isolated from an ensemble by the optical trapping technique. We show that when large size parameter spheres are used, the measured second-harmonic efficiency deviates strongly from the prediction of the nonlinear Rayleigh scattering theory. Our results are in very good agreement with the predictions from the exact nonlinear Mie scattering theory.