Abstract
Material design concept of polymeric materials applicable for 3rd-order nonlinear optical devices is reviewed. Firstly, the importance of distinguishing molecular origins for high 3rd-order optical nonlinearity is stressed. Molecular structures and preparation methods of majorπ-conjugated polymer films with potentially high optical nonlinearity are introduced. Then, relations between molecular structures and 3rd-order nonlinear susceptibilities are discussed. Stress is put on coherent 3rd-order nonlinearity, which can be examined with nonlinear sus-ceptibility spectra obtainable from third-harmonic generation experiments.