论文标题

使用DNA折纸胶体的几何编程的自限制小管组装

Geometrically programmed self-limited assembly of tubules using DNA origami colloids

论文作者

Hayakawa, Daichi, Videbæk, Thomas E., Hall, Douglas M., Fang, Huang, Sigl, Christian, Feigl, Elija, Dietz, Hendrik, Fraden, Seth, Hagan, Michael F., Grason, Gregory M., Rogers, W. Benjamin

论文摘要

自组装是在纳米级制造功能材料的最有希望的策略之一,但是需要新的设计原则,用于制造自限制体系结构,而不是空间无限的周期性晶格结构。为了应对这一挑战,我们探讨了特定类别的自限制结构的可寻址组装与自闭合组装之间的权衡:圆柱小管。我们使用具有特定的价值相互作用并设计结合角的DNA折纸制作三角亚基,并将其组装成具有比单个亚基大小大得多的自限宽度的小管。在最简单的情况下,小管是通过对相邻亚基之间的二面角编程来从单个组件组装的。我们表明,小管可以达到许多微米的长度,并且可以通过二面角开出它们的平均宽度。我们发现,小管的宽度和手性有一个分布,我们通过开发一个模型来合理化该模型,该模型考虑了组装结构的有限弯曲刚度以及自闭合的机制。最后,我们证明可以通过增加亚基物种的数量来进一步雕刻小管的分布,从而提高组装复杂性,并证明使用两个亚基物种成功地将可用终端状态的数量成功降低了一半。这些结果有助于阐明组装复杂性和几何形状在自限制组装中的作用,并且可以扩展到其他自限制体系结构,例如壳,环形或三个周期性的框架。

Self-assembly is one of the most promising strategies for making functional materials at the nanoscale, yet new design principles for making self-limiting architectures, rather than spatially unlimited periodic lattice structures, are needed. To address this challenge, we explore the trade-offs between addressable assembly and self-closing assembly of a specific class of self-limiting structures: cylindrical tubules. We make triangular subunits using DNA origami that have specific, valence-limited interactions and designed binding angles, and study their assembly into tubules that have a self-limited width that is much larger than the size of an individual subunit. In the simplest case, the tubules are assembled from a single component by geometrically programming the dihedral angles between neighboring subunits. We show that the tubules can reach many micrometers in length and that their average width can be prescribed through the dihedral angles. We find that there is a distribution in the width and the chirality of the tubules, which we rationalize by developing a model that considers the finite bending rigidity of the assembled structure as well as the mechanism of self-closure. Finally, we demonstrate that the distributions of tubules can be further sculpted by increasing the number of subunit species, thereby increasing the assembly complexity, and demonstrate that using two subunit species successfully reduces the number of available end states by half. These results help to shed light on the roles of assembly complexity and geometry in self-limited assembly and could be extended to other self-limiting architectures, such as shells, toroids, or triply-periodic frameworks.

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