1 November 1996 Structure/quadratic hyperpolarizability correlation: solvent effect
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Abstract
In this work, we have investigated theoretically the structure/hyperpolarizability correlations of push-pull molecules sing a two-form two-state model. For this, we have defined a parameter MIX characterizing the mixing between the two-limiting resonance forms and thus ruling the molecular structure and polarization. Also, we have analyzed the solvent effect on the structure and on the polarizabilities of push-pull molecules using the Onsager reaction field theory. We have shown that the dependences of the linear and nonlinear polarizabilities on the solvent dielectric constant look similar to the structure/(hyper)polarizability correlations. Finally, we have investigated experimentally the solvent effect on a series of push-pull polyenes of increasing length. In particular, we have determined the scalar (mu) g(Beta) (0) product (where (mu) g is the ground-state dipole and (Beta) (0) the vector part of static quadratic hyperpolarizability tensor) in different solvents using the electric-field-induced-second-harmonic generation technique. For the different chain lengths, we have obtained a mapping of the positive (mu) g(Beta) (0) peak. This leads for the longest compound of the series to a record high value of (mu) g(Beta) (0) product in chloroform.
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Marguerite Barzoukas, Jacques Muller, Alain F. Fort, Seth R. Marder, Valerie Alain, Mireille H. Blanchard-Desce, "Structure/quadratic hyperpolarizability correlation: solvent effect", Proc. SPIE 2852, Nonlinear Optical Properties of Organic Materials IX, (1 November 1996); doi: 10.1117/12.256168; https://doi.org/10.1117/12.256168
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