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Abstract
Third-order optical nonlinearity was investigated in two charge-transfer (CT)-type conjugated polymers, poly(aryleneethynylene) and poly(thiophene-alt-thiazole), using the third-harmonic generation (THG) method. Comparison of the results with previously obtained THG data for polythiophene and the strong CT polymer poly(thiophene-alt-quinoxaline) revealed that the ratio of the maximum value of third-order nonlinear susceptibility and the absorption coefficient max∣χ(3)∣∕αmax increased as the degree of CT character increased for the four polymers. This variation in max∣χ(3)∣∕αmax is discussed based on the magnitude of the transition dipole moment between the one-photon-allowed and the one-photon-forbidden excited states.
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