Synthesis and characterization of second- and third-order nonlinear optical materials

Organic nonlinear optical (NLO) materials have been studied for almost three decades. In that time the understanding of structure-property relationships have led to the production of materials with new capabilities and the application of those materials in other scientific disciplines. Challenges remain, however, in the fundamental design of NLO materials. Reducing the effects of electrostatic interactions between dipolar chromophores is a difficult problem. Molecules can be made by trial and error, but it is costly and time consuming. Modifying the donors and acceptors of chromophores requires characterization studies to determine the effectiveness. New chromophores that produce high beta values don't always produce bulk materials with large r33 values. More recently, theoretical calculations and insights have helped guide the synthesis of second-order NLO materials. This dissertation includes the first production of the triphenylamine donor molecule that is in wide use. It also includes Teng-Man (TM) and modified attenuated total reflection (ATR) studies on chromophores with modifications to the donor, which validated theoretical predictions. Similar TM and ATR studies revealed a promising new class of binary chromophore blends to help overcome electrostatic interaction challenges. Finally, third-order electro-optic molecules were used for two-photon absorption studies of bilipid vesicle photolysis.