Engineering of Acentric Stilbazolium Salts with Large Second-Order Optical Nonlinearity and Enhanced Environmental Stability

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• 作者：Zhihua Sun ; Xitao Liu ; Xinqiang Wang ; Lina Li ; Xiaojun Shi ; Shigeng Li ; Chengmin Ji ; Junhua Luo ; Maochun Hong
• 刊名：Crystal Growth & Design
• 出版年：2012
• 出版时间：December 5, 2012
• 年：2012
• 卷：12
• 期：12
• 页码：6181-6187
• 全文大小：483K
• 年卷期：v.12,no.12(December 5, 2012)
• ISSN：1528-7505

文摘

A series of organic nonlinear optical (NLO) materials based on the stilbazolium derivatives of 4-N,N-dimethylamino-4鈥?N鈥?methyl-stilbazolium tosylate (DAST) were synthesized, and the single crystals were grown from the solutions. Single-crystal structure determinations and Kurtz powder tests reveal that replacement of the p-toluenesulfonate anion in the DAST crystal, forming 4-N,N-dimethylamino-4鈥?N鈥?methyl-stilbazolium 4-aminotoluene-3-sulfonate (1) and 4-N,N-dimethylamino-4鈥?N鈥?methyl-stilbazolium p-chlorobenzenesulfonate (2), constructs new acentric crystals with quite a large powder second-harmonic generation (SHG) of more than 3 orders of magnitude larger than that of urea around 2.0 渭m, whereas the other two complexes show their centrosymmetric structures without any SHG effects. A possible estimation of the molecular first hyperpolarizabilities 尾_ijk performed on 2 further confirms its origin of its enhanced NLO merits. Furthermore, both 1 and 2 exhibit even higher environmental stabilities, including the antiwater performance and the formation of anhydrous phases in water-containing solutions. We believe that the findings of the further counterion modification will bring new stilbazolium derivatives with improved optical nonlinearities and the physicochemical performances.