Design of Chemoresponsive Liquid Crystals through Integration of Computational Chemistry and Experimental Studies
Design of Chemoresponsive Liquid Crystals through Integration of Computational Chemistry and Experimental Studies
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DOI：
10.1021/acs.chemmater.6b05430
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发表时间：
2017-04
影响因子：
8.6
通讯作者：
Tibor Szilvási;Luke T. Roling;Huaizhe Yu;Prabin Rai;Sang-Wook Choi;R. Twieg;M. Mavrikakis;N. Abbott
中科院分区：
文献类型：
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作者：
Tibor Szilvási;Luke T. Roling;Huaizhe Yu;Prabin Rai;Sang-Wook Choi;R. Twieg;M. Mavrikakis;N. Abbott
我们报告了使用计算化学方法来设计化学响应液晶（LC）。具体来说，我们使用电子结构计算来模拟含腈介晶（4'-n-戊基-4-联苯甲腈）与金属高氯酸盐（明确描述高氯酸根阴离子）的结合，我们将其称为配位饱和阴离子模型（CSAM）。模型结果根据实验数据进行了验证。然后，我们使用 CSAM 预测选择性氟化可以降低含腈向列液晶与金属盐修饰表面的结合强度，从而响应甲基膦酸二甲酯 (DMMP) 的竞争性结合，产生液晶的更快重新排序。我们通过合成氟化化合物 3-氟-4'-戊基[1,1'-联苯]-4-甲腈和 4-氟-4'-戊基-1,1'-联苯，并随后实验测量含有这些化合物的液晶对 DMMP 的取向响应来测试这一预测。这些实验...
We report the use of computational chemistry methods to design a chemically responsive liquid crystal (LC). Specifically, we used electronic structure calculations to model the binding of nitrile-containing mesogens (4′-n-pentyl-4-biphenylcarbonitrile) to metal perchlorate salts (with explicit description of the perchlorate anion), which we call the coordinately saturated anion model (CSAM). The model results were validated against experimental data. We then used the CSAM to predict that selective fluorination can reduce the strength of binding of nitrile-containing nematic LCs to metal-salt-decorated surfaces and thus generate a faster reordering of the LC in response to competitive binding of dimethylmethylphosphonate (DMMP). We tested this prediction via synthesis of fluorinated compounds 3-fluoro-4′-pentyl[1,1′-biphenyl]-4-carbonitrile and 4-fluoro-4′-pentyl-1,1′-biphenyl, and subsequent experimental measurements of the orientational response of LCs containing these compounds to DMMP. These experiment...