Light generation at the anomalous dispersion high energy range of a nonlinear opal film.

We study experimentally and theoretically light propagation and generation at the high energy range of a close-packed fcc photonic crystal of polystyrene spheres coated with a nonlinear material. We observe an enhancement of the second harmonic generation of light that may be explained on the basis of amplification effects arising from propagation at anomalous group velocities. Theoretical calculations are performed to support this assumption. The vector KKR method we use allows us to determine, from the linear response of the crystal, the behavior of the group velocity in our finite photonic structures when losses introduced by absorption or scattering by defects are taken into account assuming a nonzero imaginary part for the dielectric constant. In such structures, we predict large variations of the group velocity for wavelengths on the order or smaller than the lattice constant of the structure, where an anomalous group velocity behavior is associated with the flat bands of the photonic band structure. We find that a direct relation may be established between the group velocity reduction and the enhancement of a light generation processes such as the second harmonic generation we consider. However, frequencies for which the enhancement is found, in the finite photonic crystals we use, do not necessarily coincide with the frequencies of flat high energy bands.

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.