The production of coherent blue radiation with compact solid-state devices is of great technological importance for optical data storage, xerography, and spectroscopy. A viable alternative to direct lasing is second-harmonic generation (SHG), which utilizes second-order nonlinear optical (NLO) properties of the medium to convert fundamental wavelength into second-harmonic. The main requirement for creating second-order nonlinear response in a material system is noncentrosymmetric ordering on both the microscopic and the macroscopic levels. Ionic self-assembled monolayers (ISAM) technique is explored in this thesis as a method of fabricating organic thin films that possess non-zero second-order response. Numerous ISAM structures have been fabricated and characterized in this work. Publishable experimental results have been obtained using pyrylium salt dye as an NLO-active component, which is novel for ISAM applications. Waveguide geometry is employed to obtain large intensity of the fundamental beam from a low-power source, needed for efficient nonlinear interactions. Phase matching is a critical parameter for SHG. Anomalous-dispersion phase matching (ADPM) is investigated in this thesis in an attempt to demonstrate, for the first time, ADPM second-harmonic generation in an ISAM waveguide. |