Self-Assembly and Crystallization of DNA-Coated Colloids via Linker-Encoded Interactions
Self-Assembly and Crystallization of DNA-Coated Colloids via Linker-Encoded Interactions
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DOI：
10.1021/acs.langmuir.9b03391
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发表时间：
2020-06-30
期刊：
影响因子：
3.9
通讯作者：
Rogers, W. Benjamin
中科院分区：
文献类型：
--
作者：
Lowensohn, Janna;Hensley, Alexander;Rogers, W. Benjamin
用DNA包覆胶体颗粒是一种很有前途的制造功能性纳米材料的策略，因为颗粒可以被编程自发地自组装成复杂的有序结构。在这篇文章中，我们探讨了相行为和类型的结构，可以形成时，DNA包被的胶体之间的相互作用是由分散在溶液中的连接DNA链指定。我们表明，连接介导的相互作用指导胶体的自组装成平衡晶体结构。此外，我们展示了不同的连接体序列和浓度如何产生不同的晶格，其对称性和组成顺序完全由连接体介导的相互作用编码。这些结果说明了如何使用接头将编码在接头中的组装指令与胶体本身分开。我们还研究了相行为的不对称连接，更强烈地结合到一个胶体物种比其他。我们发现，不对称性强烈影响的浓度依赖性的胶体相互作用，我们解释使用平均场模型。我们还发现证据表明，不对称连接可能有助于减少动力学瓶颈胶体结晶。总之，我们的研究结果扩展了连接子介导的自组装的设计规则，并在文献中报道的DNA涂层胶体的编程组装的各种方案之间建立了联系。
Coating colloidal particles with DNA is a promising strategy to make functional nanoscale materials because the particles can be programmed to spontaneously self-assemble into complex, ordered structures. In this Article, we explore the phase behavior and types of structures that can be formed when interactions between DNA-coated colloids are specified by linker DNA strands dispersed in solution. We show that linker-mediated interactions direct the self-assembly of colloids into equilibrium crystal structures. Furthermore, we demonstrate how different linker sequences and concentrations produce different crystal lattices, whose symmetry and compositional order are encoded exclusively by the linker-mediated interactions. These results illustrate how linkers can be used to separate the assembly instructions, encoded in the linkers, from the colloids themselves. We also examine the phase behavior of asymmetric linkers, which bind more strongly to one colloidal species than the other. We find that asymmetry strongly influences the concentration dependence of the colloidal interactions, which we explain using a mean-field model. We also find evidence that asymmetric linkers might help to reduce kinetic bottlenecks to colloidal crystallization. Together, our findings expand the design rules of linker-mediated self-assembly and make connections between the various schemes for programming assembly of DNA-coated colloids reported in the literature.