1 December 1991 Design of chromophores for nonlinear optical applications
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In designing chromophores for second harmonic generation applications one would like to have a large hyperpolarizability (beta) and an absorption well away from the second harmonic frequency. Unfortunately, there appears to be a connection between the experimentally observed absorption maximum energy and the observed zero-frequency hyperpolarizability (beta) 0, when comparing different molecules within a class, such as donor/acceptor substituted benezenes and stilbenes, that makes this difficult to achieve. In this paper, the origins of this relationship are investigated by comparing results from semi-empirical calculations with experimental values. A significant contribution to the observed relationship between absorption maximum and (beta) 0 is seen to arise from frequency dependences of the ground and excited state dipole moments. Since the two-level model for (beta) is used both as an extrapolation technique to obtain (beta) 0 and as a tool for analyzing the data, a discussion of the validity of this model is also presented.
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Donald M. Burland, Donald M. Burland, J. E. Rice, J. E. Rice, John Downing, John Downing, Josef Michl, Josef Michl, "Design of chromophores for nonlinear optical applications", Proc. SPIE 1560, Nonlinear Optical Properties of Organic Materials IV, (1 December 1991); doi: 10.1117/12.50710; https://doi.org/10.1117/12.50710

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