Modeling of configurations and third-order nonlinear optical properties of methyl silsesquioxanes

J. Shen, W. D. Cheng, D. S. Wu, X. D. Li, Y. Z. Lan, H. Zhang, Y. J. Gong, F. F. Li, S. P. Huang

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Abstract

Configuration optimizations, excited state properties, and the frequency-dependent third-order nonlinear optical polarizabilities have been investigated on a series of methyl-silsesquioxane (MeT) cages [C H3 Si O1.5] n (n=4, 6, 8, and 10) using ab initio quantum mechanical methods coupled with the sum-over-states methods. The obtained electronic absorption spectra show a redshift as the cage size increases, and the absorption spectra are assigned as charge transfers from oxygen p type to silicon s type atomic orbitals. The calculated average third-order polarizabilities of 〈γ〉 in the three optical physical processes (third-harmonic generation, the electric-field-induced second-harmonic generation, and degenerate four-wave mixing) have wide nonresonance regions. For all the considered species, the values of γ decrease in the order of [MeT]4>[MeT]8 (C2v) = [MeT]10>[MeT]6>[MeT]8 (Oh).

Original languageEnglish (US)
Article number204709
JournalJournal of Chemical Physics
Volume122
Issue number20
DOIs
StatePublished - May 22 2005

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    Shen, J., Cheng, W. D., Wu, D. S., Li, X. D., Lan, Y. Z., Zhang, H., Gong, Y. J., Li, F. F., & Huang, S. P. (2005). Modeling of configurations and third-order nonlinear optical properties of methyl silsesquioxanes. Journal of Chemical Physics, 122(20), [204709]. https://doi.org/10.1063/1.1913528