Contraction and Expansion of Stimuli-Responsive DNA Bonds in Flexible Colloidal Crystals
Contraction and Expansion of Stimuli-Responsive DNA Bonds in Flexible Colloidal Crystals
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DOI：
10.1021/jacs.6b05430
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发表时间：
2016-07-20
影响因子：
15
通讯作者：
Mirkin, Chad A.
中科院分区：
文献类型：
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作者：
Mason, Jarad A.;Laramy, Christine R.;Mirkin, Chad A.
DNA表面配体可以作为可编程的“键”来控制纳米颗粒在晶体超晶格中的排列。在这里，我们研究了这些DNA键对局域介电常数(epsilon(R))变化的内在响应性，作为一种动态调制超晶格结构的新方法。值得注意的是，乙醇(Etoh)的加入可以用来可控地调节DNA键长从16到3 nm，并将键的稳定性提高>；40℃，同时保持长程有序和结晶习惯。有趣的是，我们发现这些结构变化，其中包括晶体体积的膨胀和收缩高达75%，一旦达到临界比例的乙醇，就会以一种协同的方式发生。这些结果提供了一种简单而稳健的方法来创建刺激响应晶格，获得高体积分数，并提高热稳定性。
DNA surface ligands can be used as programmable "bonds" to control the arrangement of nanoparticles into crystalline superlattices. Here, we study the intrinsic responsiveness of these DNA bonds to changes in local dielectric constant (epsilon(r)) as a new approach to dynamically modulate superlattice structure. Remarkably, ethanol (EtOH) addition can be used to controllably tune DNA bond length from 16 to 3 nm and to increase bond stability by >40 degrees C, while retaining long-range order and crystal habit. Interestingly, we find that these structural changes, which involve the expansion and contraction of crystals by up to 75% in volume, occur in a cooperative fashion once a critical percentage of EtOH is reached. These results provide a facile and robust approach to create stimuli-responsive lattices, to access high volume fractions, and to improve thermal stability.