Electronic structure and nonlinear optical properties of push-pull polyenes: theoretical investigation of benzodithia polyenals and dithiolene polyenals

A comprehensive theoretical characterization of the geometric structure, electronic properties and first- and second order polarizibilities of a series of push-pull polyene molecules is performed by ab initio Hartree-Fock approximations. The results indicate that the geometric structure of the polyenic segment is independent of the presence of the donor acceptor groups. It is observed that the average first-order polarizabilities are of the same order of magnitude for the compounds under consideration.