The principal focus of the project is to develop new materials chemistry based on molecular level design and solid state chemistry. The goals have been to develop electroactive polymers with novel electronic, optical and nonlinear optical properties. Second and third order nonlinear optical materials have been developed based on conjugated macromolecules and asymmetric anharmonic molecular electronic dipolar oscillators. In this multidisciplinary research effort, starting from the first principle, polymeric systems have been developed with stable large nonlinear optical coefficients, ultrathin electroactive redox monolayers, molecular superlattices, and others. Sol-gel chemistry, photochemical crosslinking and photopolymerization have been employed as engineering tools in materials fabrication and to elicit new phenomenon.