This project is aimed at determining the dynamics of third-order nonlinear optical processes in molecular and polymeric materials. Research to be undertaken will include: degenerate four-wave mixing and two-wave mixing pump-probe experiments using amplified 60 femtosecond pulses; investigating the role of two-photon absorption, bimolecular decay, and excitation saturation by simultaneously monitoring both first-order and higher-order diffractions during degenerate four-wave mixing; observing the relative roles of initially photogenerated excitons and subsequently formed polarons in determining optical nonlinearity in linear conjugated structures.