Calculation of hyperpolarizabilities of TTF-derived chromophores

Molecular orbital calculations have been performed at semiempirical and ab initio levels to evaluate the second order nonlinear optical properties of a series of chromophores containing tetrathiafulvalene and different acceptor moieties. Semiempirical (AMI and PM3) and ab initio (CPHF/6-31G*) calculations are compared to experimental (EFISH) values in order to evaluate the predictive power of these theoretical methods.