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The Relationship Between Second-Order Nonlinear Optical Properties And Ground-State Polarization

Published online by Cambridge University Press:  16 February 2011

Grant Bourhill,
Lap-Tak Cheng,
Ging Lee,
Seth R. Marder,
Joseph W. Perry,
Matthew J. Perry and
Bruce G. Tiemann
Grant Bourhill
Affiliation:
Jet Propulsion Laboratory, 67–201, California Institute of Technology, Pasadena, CA 91109.
Lap-Tak Cheng
Affiliation:
Central Research and Development, Science and Engineering Laboratories, E. I. Du Pont de Nemours & Co. (Inc.), Experimental Station, P. O. Box 80356, Wilmington, DE 19880.
Ging Lee
Affiliation:
The Beekman Institute, 139–74, California Institute of Technology, Pasadena, CA 91125.
Seth R. Marder
Affiliation:
Jet Propulsion Laboratory, 67–201, California Institute of Technology, Pasadena, CA 91109.The Beekman Institute, 139–74, California Institute of Technology, Pasadena, CA 91125.
Joseph W. Perry
Affiliation:
Jet Propulsion Laboratory, 67–201, California Institute of Technology, Pasadena, CA 91109.
Matthew J. Perry
Affiliation:
The Beekman Institute, 139–74, California Institute of Technology, Pasadena, CA 91125.
Bruce G. Tiemann
Affiliation:
Jet Propulsion Laboratory, 67–201, California Institute of Technology, Pasadena, CA 91109.The Beekman Institute, 139–74, California Institute of Technology, Pasadena, CA 91125.
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Abstract

A review is presented describing our recent work to correlate the first hyperpolarizability, β, of organic materials with the molecular parameter bond length alternation (BLA). Donor-acceptor polyenes displaying a wide BLA range were synthesized. For a particular chromophore, BLA was fine-tuned by varying solvent polarity. The degree of BLA was analyzed by X-ray diffraction, 1H-NMR and electronic absorption spectroscopy. Non-resonant, solvent-dependent, electric field induced second harmonic generation (EFISH) Measurements were performed to probe the variation in the second-order nonlinearity as a function of ground-state polarization. The resulting trend, which is fully consistent with theoretical predictions, identified chromophores possessing optimized positive and negative hyperpolarizabilities. An optimized chromophore was incorporated in a polymer matrix and poled. The resulting electro-optic coefficient was found to be significantly enhanced relative to the longer chromophore Disperse Red 1.

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References

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