Design of Polymethine Dyes with Large Third-Order Optical Nonlinearities and Loss Figures of Merit

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 (γ) 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 γ. We implemented this strategy in a soluble bis(selenopyrylium) heptamethine dye that exhibits a real part of γ that is exceptionally large throughout the wavelength range used for telecommunications, and an imaginary part of γ, 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.