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Science. 2010 Mar 19;327(5972):1485-8. doi: 10.1126/science.1185117. Epub 2010 Feb 18.

Design of polymethine dyes with large third-order optical nonlinearities and loss figures of merit.

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School of Chemistry and Biochemistry and Center for Organic Photonics and Electronics, Georgia Institute of Technology, Atlanta, GA 30332, USA.


All-optical switching applications require materials with large third-order nonlinearities and low nonlinear optical losses. We present a design approach that involves enhancing the real part of the third-order polarizability (gamma) of cyanine-like molecules through incorporation of polarizable chalcogen atoms into terminal groups, while controlling the molecular length to obtain favorable one- and two-photon absorption resonances that lead to suitably low optical loss and appreciable dispersion enhancement of the real part of gamma. We implemented this strategy in a soluble bis(selenopyrylium) heptamethine dye that exhibits a real part of gamma that is exceptionally large throughout the wavelength range used for telecommunications, and an imaginary part of gamma, a measure of nonlinear loss, that is smaller by two orders of magnitude. This combination is critical in enabling low-power, high-contrast optical switching.

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