The nonlinear optical properties of organics with unsaturated bonds were compared with those of inorganics including semiconductors and dielectrics. Because of the mesomeric effect, namely quantum mechanical resonance effect among configurations, aromatic molecules and polymers have larger optical nonlinear parameters defined as δ(n)=X(n)/(X(l))n both for the second (n=2) and third-order (n=3) nonlinearities. Experimental results of ultrafast nonlinear response of conjugated polymers, especially polydiacetylenes, were described and a model is proposed to explain the relaxation processes of photoexcitations in the conjugated polymers. Applying the model constructed on the basis of the extensive experimental study, we propose model polymers to obtain ultrafast resonant optical nonlinearity.

The nonlinear optical properties of organics with unsaturated bonds were compared with those of inorganics including semiconductors and dielectrics. Because of the mesomeric effect, namely quantum mechanical resonance effect among configurations, aromatic molecules and polymers have larger optical nonlinear parameters defined as δ(n)X(n)/(X(1))n both for the second (n2) and third-order (n3) nonlinearities. Experimental results of ultrafast nonlinear response of conjugated polymers, especially polydiacetylenes, were described and a model is proposed to explain the relaxation processes of photoexcitations in the conjugated polymers. Applying the model constructed on the basis of the extensive experimental study, we propose model polymers to obtain ultrafast resonant optical nonlinearity.