Resonance-enhanced Second Harmonic Generation from spherical microparticles in aqueous suspension

• Main Author: Viarbitskaya, Sviatlana
• Format: Doctoral Thesis
• Language: English
• Published: Stockholm University, Faculty of Science, AlbaNova University Center (together with KTH) 2008
• Subjects: Nonlinear optics; second harmonic generation; adsorption; molecules; Physics; Fysik
• Online Access: http://urn.kb.se/resolve?urn=urn:nbn:se:su:diva-7517; http://nbn-resolving.de/urn:isbn:978-91-7155-665-3

Second harmonic generation (SHG) is a nonlinear optical effect sensitive to interfaces between materials with inversion symmetry. It is used as an effective tool for detection of the adsorption of a substance to microscopic particles, cells, liposomes, emulsions and similar structures, surface analysis and characterization of microparticles. The scattered second harmonic (SH) intensity from surfaces of suspended microparticles is characterized by its complex angular distribution dependence on the shape, size, and physical and chemical properties of the molecules making up the outer layer of the particles. In particular, the overall scattered SH intensity has been predicted to have a dramatic and nontrivial dependence on the particle size. Results are reported for aqueous suspensions of polystyrene microspheres with different dye molecules adsorbed on their surfaces. They indicate that the scattered SH power has an oscillatory dependence on the particle size. It is also shown that adsorption of one of the dyes (malachite green) on polystyrene particles is strongly affected when SDS surfactants are added to the solution. For this system a rapid increase of the SH signal with increasing concentration of SDS was observed in the range of low SDS concentration. Three different theoretical models are used to analyze the observed particle size dependence of SHG. The calculated angular and particle size dependences of the SH scattered power show that the models do not agree very well between each other when the size of the particles is of the order of the fundamental light wavelength, as here. One of the models - nonlinear Mie scattering - predicts oscillatory behaviour of the scattered SH power with the particle size, but fails to reproduce the position of the maxima and minima of the experimentally observed oscillations. The obtained results on the size dependence of the SH can be used in all applications to increase the count rate by choosing particles of the size for which the SH efficiency was found to the highest. A new effect of cooperative malachite green and SDS interaction at the polystyrene surface can be employed, for example, in the areas of microbiology or biotechnology, where adsorption macromolecules, surfactants and dyes to polystyrene microparticles is widely used.