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Science 29 July 1994:
Vol. 265. no. 5172, pp. 632 - 635
DOI: 10.1126/science.265.5172.632
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Articles

A Unified Description of Linear and Nonlinear Polarization in Organic Polymethine Dyes

Seth R. Marder 1, Christopher B. Gorman 1, Fabienne Meyers 2, Joseph W. Perry 1, Grant Bourhill 3, Jean-Luc Brédas 4, and Brian M. Pierce 5

1 Jet Propulsion Laboratory, California Institute of Technology, Pasadena, CA 91109, and Molecular Materials Resource Center, Beckman Institute, California Institute of Technology, Pasadena, CA 91125, USA.
2 Center for Research on Molecular Electronics and Photonics, Université de Mons-Hainaut, Place du Parc 20, B-7000 Mons, Belgium, and Molecular Materials Resource Center, Beckman Institute, California Institute of Technology, Pasadena, CA 91125, USA.
3 Jet Propulsion Laboratory, California Institute of Technology, Pasadena, CA 91109, USA.
4 Center for Research on Molecular Electronics and Photonics, Université de Mons-Hainaut, Place du Parc 20, B-7000 Mons, Belgium
5 Hughes Aircraft Company, Radar Systems, Building R2, MS V518, Post Office Box 92426, Los Angeles, CA 90009, USA.

An internal or external electric field F can drive the chemical structure, bond order alternation, and electronic structure of linear polymethine dyes from a neutral, bond-alternated, polyene-like structure, through a cyanine-like structure, and ultimately to a zwitterionic (charge-separated) bond-alternated structure. As the structure evolves under the influence of F, the linear polarizability agr, the first hyperpolarizability beta, and the second hyperpolarizability ggr are seen to be derivatives, with respect to F, of their next lower order polarization (for agr) or polarizability (for beta and ggr). These derivative relations provide a unified picture of the dependence of the polarizability and hyperpolarizabilities on the structure in linear polymethine dyes. In addition, they allow for predictions of structure-property relations of higher order hyperpolarizabilities.

Submitted on March 1, 1994
Accepted on June 6, 1994


THIS ARTICLE HAS BEEN CITED BY OTHER ARTICLES:
Low (Sub-1-Volt) Halfwave Voltage Polymeric Electro-optic Modulators Achieved by Controlling Chromophore Shape.
Y. Shi, C. Zhang, H. Zhang, J. H. Bechtel, L. R. Dalton, B. H. Robinson, and W. H. Steier (2000)
Science 288, 119-122
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