Self-Assembly of All-DNA Rods with Controlled Patchiness
Self-Assembly of All-DNA Rods with Controlled Patchiness
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DOI：
10.1002/smll.202104510
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发表时间：
2021-11-27
期刊：
影响因子：
13.3
通讯作者：
Stiakakis, Emmanuel
中科院分区：
文献类型：
--
作者：
Gvozden, Katarina;Ratajczak, Sanja Novak;Stiakakis, Emmanuel
双链DNA（dsDNA）片段在其尖端之间表现出非共价吸引相互作用。目前还不清楚DNA液晶自组装是如何受到这种平端吸引力的影响的。结果表明，在选择性筛选平端DNA堆积相互作用的基础上，具有中等长径比的刚性dsDNA片段可以在浓水溶液中特异性地自组装成不同类型的近晶相.为此，通过构建DNA双链体在分子水平上对这种类型的吸引力进行工程改造，其中一端或两端之间的吸引力通过短发夹帽进行筛选。全DNA双层和单层近晶-A型相，以及柱状相，可以通过控制吸引强度来稳定。结果表明，迄今为止，在DNA棒状液晶中难以捉摸的近晶-A是一个化学稳定相。双层近晶相的存在被证实的蒙特-卡罗模拟硬柱装饰一个有吸引力的终端网站。这项工作表明，DNA平端表现为定义明确的单价有吸引力的补丁，其强度和位置可以潜在地精确调整，突出了关于稳定的非传统的基于DNA的溶致液晶相组装的所有DNA补丁颗粒与任意的几何形状和组成的独特的机会。
Double-stranded DNA (dsDNA) fragments exhibit noncovalent attractive interactions between their tips. It is still unclear how DNA liquid crystal self-assembly is affected by such blunt-end attractions. It is demonstrated that stiff dsDNA fragments with moderate aspect ratio can specifically self-assemble in concentrated aqueous solutions into different types of smectic mesophases on the basis of selectively screening of blunt-end DNA stacking interactions. To this end, this type of attractions are engineered at the molecular level by constructing DNA duplexes where the attractions between one or both ends are screened by short hairpin caps. All-DNA bilayer and monolayer smectic-A type of phases, as well as a columnar phase, can be stabilized by controlling attractions strength. The results imply that the so far elusive smectic-A in DNA rod-like liquid crystals is a thermodynamically stable phase. The existence of the bilayer smectic phase is confirmed by Monte-Carlo simulations of hard cylinders decorated with one attractive terminal site. This work demonstrates that DNA blunt-ends behave as well-defined monovalent attractive patches whose strength and position can be potentially precisely tuned, highlighting unique opportunities concerning the stabilization of nonconventional DNA-based lyotropic liquid crystal phases assembled by all-DNA patchy particles with arbitrary geometry and composition.