Controlling Fragment Competition on Pathways to Addressable Self-Assembly.
Controlling Fragment Competition on Pathways to Addressable Self-Assembly.
复制标题
控制可寻址自组装途径上的片段竞争。
DOI：
10.1021/acs.jpcb.8b08096
复制
发表时间：
2018
期刊：
影响因子：
--
通讯作者：
Madge J
中科院分区：
文献类型：
--
作者：
Madge J
可寻址自组装是由一组独特的分子或胶体构建块形成目标结构，每个分子或胶体构建块占据目标中的定义位置。每种类型的构建块在目标的每个副本中仅出现一次的要求对粒子的组合以及导致成功自组装的路径产生了严格的限制。这些限制会限制自组装的效率和产品的最终产量。特别是，如果部分形成的片段的成分重叠，则它们可能会相互竞争，因为它们无法组合。在这里，我们引入了一种“可完成性”算法来量化自组装片段之间的竞争，并用它来推导出抑制小可寻址簇自组装中片段不兼容影响的一般原理。竞争源自目标结构的键合网络中的环，但可能需要环来提供结构刚性和热力学稳定性。通过仔细选择结合网络并促进排除早期片段之间竞争的半分级途径，可以实现最佳折衷。这些概念在两个对比鲜明的可寻址目标（每个目标有 20 个独特组件）的自组装模拟中得到了说明。
Addressable self-assembly is the formation of a target structure from a set of unique molecular or colloidal building blocks, each of which occupies a defined location in the target. The requirement that each type of building block appears exactly once in each copy of the target introduces severe restrictions on the combinations of particles and on the pathways that lead to successful self-assembly. These restrictions can limit the efficiency of self-assembly and the final yield of the product. In particular, partially formed fragments may compete with each other if their compositions overlap, since they cannot be combined. Here, we introduce a “completability” algorithm to quantify competition between self-assembling fragments and use it to deduce general principles for suppressing the effects of fragment incompatibility in the self-assembly of small addressable clusters. Competition originates from loops in the bonding network of the target structure, but loops may be needed to provide structural rigidity and thermodynamic stability. An optimal compromise can be achieved by careful choice of bonding networks and by promoting semihierarchical pathways that rule out competition between early fragments. These concepts are illustrated in simulations of self-assembly in two contrasting addressable targets of 20 unique components each.
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