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 , the rotational average of the third-order molecular polarizability is for the best molecule, which corresponds to 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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