Abstract

AbstractAs new ionic organic species for second‐order non‐linear optical (NLO) materials, 4‐{[4‐(dimethylamino)phenyl]ethynyl}phenyltrimethylammonium iodide (1a), 4‐{[4‐(dimethylamino)phenyl]butadiynyl}phenyltrimethylammonium iodide (2a) and their derivatives with 4‐substituted benzensulfonate instead of iodide were successfully synthesized. The transparent wavelength region of 1a is wider than that of a typical NLO molecule, p‐nitroaniline (pNA), whereas 2a and pNA have similar transparent regions. The experimental and calculated first hyperpolarizabilities (β) of 1a and 2a were found to be about 7 and 11 times, respectively, larger than those of pNA. Even when the volume factor was taken into account, the cationic part of 1a was found to be a better second‐order NLO material than pNA derivatives. Four second‐order NLO‐active crystals were found out of 12 salts synthesized. Copyright © 2004 John Wiley & Sons, Ltd.

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