Ab initio predictions of large hyperpolarizability push-pull polymers. Julolidinyl-n-isoxazolone and julolidinyl-n-N,N′-diethylthiobarbituric acid

Recently significant advances have been made in engineering push-pull organic chromophores to have very large hyperpolarizabilities ( β ), leading to materials with μβ as high as 15000 X 10−48 esu. Such developments have been slow and costy because of difficulties in synthesis, purification, and measurement. As an alternative we have developed a new quantum mechanical program (PS-GVB/NLO) which provides predictions of β for such molecules far faster preeviously possible. We have applied PS-GVB/NLO to predicting a, β, and γ for the high β push-pull organics and find excellent agreement with experiment. This suggests that theory can be used as an effective tool for developing new nonlinear optical materials.