ABSTRACTNew polymers incorporating a variety of electroactive moeities with defined π-electron conjugation lengths have been synthesized and characterized by degenerate four wave mixing (DFWM) techniques. The χ(3)/α values for these materials varied from 10−12 to 10−13 esu cm. This work has identified several promising structures with nonlinear optical activity including organometallic and purely organic materials. The preparation of composite materials has also permitted the measurement of χ(3)/α as a function of the electroactive unit concentration.