A comparative study of the second-harmonic efficiency of monomolecular coverages of organic dyes has been performed. Although a simple excitation geometry has been used, the study reveals important relations among orientation, chemical structure, and nonlinear polarizability. In particular, pyridine compounds of appropriate chain length show a high hyperpolarizability α¯¯(2) and also a high nonlinear surface polarizability χ¯¯s(2) owing to regular self-alignment.
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Marowsky et al. (1987) studied this question.
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