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Dispersion of the third-order susceptibility of a cyanine dye measured by coherent anti-Stokes Raman scattering

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Abstract

The dispersion of the third-order susceptibility of the cyanine dye bis-(dimethylamino)-heptamethinium chloride was measured by Coherent Anti-Stokes Raman Scattering (CARS) over a wide wavelength range from 530 to 830 nm. Large negative values of the real part of the second-order hyperpolarizability are observed. The data are analyzed with the help of theoretical calculations based on a perturbative approach for the nonlinearities. The dispersion behavior of the third-order susceptibility is governed by the resonant enhancement due to vibrational transitions of the first excited electronic state and, to lesser extent, by an electronic two-photon resonance around 600 nm.

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Johr, T., Werncke, W., Dähne, L. et al. Dispersion of the third-order susceptibility of a cyanine dye measured by coherent anti-Stokes Raman scattering. Appl. Phys. B 63, 641–647 (1996). https://doi.org/10.1007/BF01831006

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  • DOI: https://doi.org/10.1007/BF01831006

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