## Abstract

We investigated the third-order nonlinear optical properties of several donor-substituted cyanoethynylethene molecules in the zero-frequency limit. We observed nonlinearities that are extraordinarily large relative to the small molecular mass of these molecules and that are within a factor of 50 from the fundamental limit. At a wavelength of $1.5\text{\hspace{0.17em}}\mu \mathrm{m}$, the rotational average of the third-order molecular polarizability is $53\pm 13\times {10}^{-48}\text{\hspace{0.17em}}{\mathrm{m}}^{5}\text{\hspace{0.17em}}{\mathrm{V}}^{-2}\phantom{\rule{0.3em}{0ex}}(3.8\times {10}^{-33}\text{\hspace{0.17em}}\mathrm{esu})$ for the best molecule, which corresponds to $1.7\times {10}^{-48}\text{\hspace{0.17em}}{\mathrm{m}}^{5}\text{\hspace{0.17em}}{\mathrm{V}}^{-2}$ per delocalized electron. The high nonlinear efficiency of these molecules is due to the compact two-dimensional conjugated system and the effective donor–acceptor substitution patterns.

© 2005 Optical Society of America

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