Published online by Cambridge University Press: 25 February 2011
We discuss two important aspects of the nonlinear optical response of polyacetylene, the prototype conjugated polymer. In the subband gap region, χ(3) of polyacetylene has a rich spectral response and its magnitude is found to be the largest among semiconductors. In the superband gap region, absorption of photons leads to direct photogeneration of charged solitons on a femtosecond-time-scale. These results are discussed in the context of a one-dimensional, coupled electronlattice system, and are generalized to other conjugated polymers.