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 µm, the rotational average of the third-order molecular polarizability is 53±13×10<sup>−48</sup> m<sup>5</sup> V<sup>−2</sup> (3.8×10<sup>−33</sup> esu) for the best molecule, which corresponds to 1.7×10<sup>−48</sup> m<sup>5</sup> V<sup>−2</sup> 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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