Absorption spectra and second-harmonic generation of Langmuir–Blodgett monolayers containing a hemicyanine dye with a large second-order hyperpolarizability are reported. The dye is found to be in the form of H aggregates in a pure-dye film and mostly monomeric in a 1:4 dye–arachidic acid film. This observation explains a report in the literature that mixed dye–arachidic acid films display greater second-harmonic generation efficiency than a pure-dye film. It may also be a factor in the reported failure of second-harmonic generation to increase quadratically with the number of layers in noncentrosymmetric multilayer films.
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Schildkraut et al. (1988) studied this question.
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