Angle-resolved second harmonic light scattering from colloidal suspensions and second harmonic particle microscopy

We have carried out two nonlinear optical experiments with colloidal particles. Our first nonlinear optical experiment studied Second-Harmonic Generation (SHG) light scattering from colloidal suspension. In particular, we measured the angle-resolved second-harmonic generation light scattering from suspensions of centrosymmetric micron-size polystyrene spheres with surface-adsorbed dye (malachite green). The second-harmonic scattering angular profiles differ qualitatively from the linear light scattering angular profiles of the same particles. We have investigated these radiation patterns using several polarization configurations and particle diameters. We introduce a simple Rayleigh-Gans-Debye model to account for the SHG scattering anisotropy. The model compares favorably with our experimental data. Our measurements suggest scattering anisotropy may be used to isolate particle nonlinear optical effect from other bulk nonlinear optical effects in suspension.; Our second nonlinear optical experiment studied the Second-Harmonic Generation (SHG) from single micron-size particles. We built a nonlinear optical microscope for this purpose. We report experimental observations of second harmonic generation from single micron-size polystyrene (PS), silica, and PolyMethylMethAcrylate (PMMA) spheres on flat substrates by SHG microscopy. At low input light intensities the SH signals depend quadratically on the intensity of the excitation beam, but at larger input intensities some of the SH signals increase exponentially with increasing input intensity. This exponential enhancement depends on particle size and sphere composition. We describe the experiments, report the observations and provide an approximate analytical framework for understanding our measurements.