15 May 1994 Experimental demonstration of the relationship between the second- and third-order polarizabilities of conjugated donor-acceptor molecules
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Abstract
The dependence of the second- and third-order polarizabilities ((beta) and (gamma) ) on ground-state polarization was measured for a series of donor-acceptor polyenes using electric field induced second harmonic generation and third harmonic generation, respectively. The changes in ground-state polarization, associated with the donor/acceptor strength or solvent polarity, were probed by x-ray crystallography, 1H-NMR, electronic absorption, and Raman spectroscopies. The observed behavior of (beta) and (gamma) as a function of ground- state polarization agrees well with theoretical predictions. In particular, positive and negative peaks, as well as sign changes, were observed for both (beta) and (gamma) . The dependences for (beta) and (gamma) are consistent with a derivative relationship between them. In addition, the third-order polarizability of a series of molecules possessing zero bond length alternation was found to be negative, in agreement with predictions based on the relationship between the polarizabilities and ground-state geometry.
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Grant Bourhill, Lap-Tak A. Cheng, Christopher B. Gorman, Ging Lee, Seth R. Marder, Joseph W. Perry, M. J. Perry, and Bruce G. Tiemann "Experimental demonstration of the relationship between the second- and third-order polarizabilities of conjugated donor-acceptor molecules", Proc. SPIE 2143, Organic, Metallo-Organic, and Polymeric Materials for Nonlinear Optical Applications, (15 May 1994); doi: 10.1117/12.173815; https://doi.org/10.1117/12.173815
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