Nonlinear optical properties of conjugated polymers from ab initio finite oligomer calculations

A review of our own work on ab initio calculation of nonlinear optical properties by the finite oligomer method is presented. Various computational considerations such as geometry determination and choice of basis set are discussed as well as extrapolation to the long‐chain limit. For cases where the extrapolation is problematic, two potential solutions are suggested. We also analyze several important areas ripe for investigation including the frequency‐dependence, the effect of vibrational distortion, and the role of electron correlation.