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Sequential programmable self-assembly: Role of cooperative interactions

机译：顺序可编程自组装：协作交互的作用

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摘要

We propose a general strategy of "sequential programmable self-assembly" that enables a bottom-up design of arbitrary multi-particle architectures on nano-and microscales. We show that a naive realization of this scheme, based on the pairwise additive interactions between particles, has fundamental limitations that lead to a relatively high error rate. This can be overcome by using cooperative interparticle binding. The cooperativity is a well known feature of many biochemical processes, responsible, e.g., for signaling and regulations in living systems. Here we propose to utilize a similar strategy for high precision self-assembly, and show that DNA-mediated interactions provide a convenient platform for its implementation. In particular, we outline a specific design of a DNA-based complex which we call "DNA spider," that acts as a smart interparticle linker and provides a built-in cooperativity of binding. We demonstrate versatility of the sequential self-assembly based on spider-functionalized particles by designing several mesostructures of increasing complexity and simulating their assembly process. This includes a number of finite and repeating structures, in particular, the so-called tetrahelix and its several derivatives. Due to its generality, this approach allows one to design and successfully self-assemble virtually any structure made of a "GEOMAG" magnetic construction toy, out of nanoparticles. According to our results, once the binding cooperativity is strong enough, the sequential self-assembly becomes essentially error-free. (C) 2016 AIP Publishing LLC.
机译：我们提出了“顺序可编程自组装”的通用策略，该策略可以实现纳米级和微米级任意多粒子体系结构的自底向上设计。我们表明，基于粒子之间的成对加性相互作用，该方案的幼稚实现具有导致相对较高错误率的基本限制。这可以通过使用协同粒子间结合来克服。协同作用是许多生化过程的众所周知的特征，例如，负责生物系统中的信号传递和调节。在这里，我们建议利用类似的策略进行高精度自组装，并证明DNA介导的相互作用为其实现提供了便利的平台。特别是，我们概述了基于DNA的复合物（称为“ DNA蜘蛛”）的特定设计，该复合物充当智能的粒子间连接子并提供内置的结合协同作用。我们通过设计一些复杂性不断提高的介观结构并模拟其组装过程，证明了基于蜘蛛功能化颗粒的顺序自组装的多功能性。这包括许多有限且重复的结构，特别是所谓的四螺旋及其数个导数。由于其通用性，这种方法允许人们设计并成功地使用纳米粒子从“ GEOMAG”磁性建筑玩具中制作出几乎任何结构，并对其进行自我组装。根据我们的结果，一旦绑定合作性足够强，顺序自组装就变得基本上没有错误。 （C）2016 AIP出版有限责任公司。

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