Molecular Optics: Nonlinear Optical Processes in Organic and Polymer Crystals

Abstract

Physical studies of nonlinear optical properties of organic and polymer structures have demonstrated exceptionally large second and third order nonlinear optical responses that are important to the fields of nonlinear optics and optical device technologies. These unusual responses have been exhibited by a large number of structures, phases, and states that include organic solids and films, single crystal polymers, Langmuir-Blodgett films, liquid crystals, and liquid crystal polymers. Experimental and theoretical studies of such systems have achieved significant advances in the understanding of these exceptional macroscopic nonlinear optical responses based on theoretically calculated microscopic electronic mechanisms, especially the role of electron-electron correlations and highly charge correlated electron excited states. Combined theory and experiment has led to the recent discovery of liquid crystal polymerization of divinyldiacetylene monomers to form highly conjugated liquid crystal polymers exhibiting large second and third order nonlinear optical responses.