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 (beta), leading to materials with mu beta as high as 15000 X 10(-48) esu. Such developments have been slow and costy because of difficulties in synt hesis, purification, and measurement. As an alternative we have develo ped a new quantum mechanical program (PS-GVB/NLO) which provides predi ctions of beta for such molecules far faster than previously possible. We have applied PS-GVB/NLO to predicting alpha, beta, and gamma for t he high beta push-pull organics and find excellent agreement with expe riment. This suggests that theory can be used as an effective tool for developing new nonlinear optical materials.