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Issue 10, 2012
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Polymethine dyes for all-optical switching applications: a quantum-chemical characterization of counter-ion and aggregation effects on the third-order nonlinear optical response

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Abstract

Polymethine dyes have recently demonstrated promise for all-optical switching applications at telecommunications wavelengths as they can combine large refractive optical nonlinearities with low single-photon and two-photon optical losses. Here, we use density functional theory and symmetry-adapted cluster configuration interaction calculations to characterize model streptocyanine molecules. We first consider the isolated, closed-shell cationic molecules and then complexes formed by the molecules with chloride counter-ions and a series of aggregates. Our goal is to examine the influence of: (i) the presence of counter-ions and (ii) aggregation on the electronic structure and nonlinear optical properties. We find that the counter-ions increase the degree of bond-length alternation along the cyanine backbone, while aggregation significantly reduces the energy window between the lowest one-photon and two-photon excited states. Our results provide insight toward the design of new polymethine derivatives that could maintain large figures-of-merit for all-optical switching applications in the solid state.

Graphical abstract: Polymethine dyes for all-optical switching applications: a quantum-chemical characterization of counter-ion and aggregation effects on the third-order nonlinear optical response

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Publication details

The article was received on 02 Jul 2012, accepted on 14 Jul 2012 and first published on 17 Jul 2012


Article type: Edge Article
DOI: 10.1039/C2SC20861J
Citation: Chem. Sci., 2012,3, 3103-3112
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    Polymethine dyes for all-optical switching applications: a quantum-chemical characterization of counter-ion and aggregation effects on the third-order nonlinear optical response

    S. Mukhopadhyay, C. Risko, S. R. Marder and J. Brédas, Chem. Sci., 2012, 3, 3103
    DOI: 10.1039/C2SC20861J

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