Organic electrooptical (EO) chromophores are now gaining more attention because the property of organic photorefrative (PR) materials could be controlled by doped EO chromophores. The new optimized chromophores were successfully implemented into PR polymers and lead to materials with substantially increased dynamic range. In this paper, electronic and nonlinear optical (NLO) properties of a new group of organic electrooptical chromophores, synthesized recently in our laboratory, were elucidated theoretically with the semiemperical quantum chemical theory. The electronic transition intensity, dipole moment and the second-order polarizability were obtained. The results show this group of chromophores possess appropriate optical absorption property, good electrooptical property and optical activity. The second-order polarizabilities β are as large as the order of 10−29 to 10−28 ESU, indicating the promising applications in the future. The physical mechanism of NLO is discussed by means of molecular orbital and electronic charge distribution.

© 2005 Optical Society of America

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