Seeding the Self-Assembly of DNA Origamis at Surfaces
Seeding the Self-Assembly of DNA Origamis at Surfaces
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在表面播种 DNA 折纸的自组装
DOI：
10.1021/acsnano.9b09348
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发表时间：
2020
期刊：
影响因子：
17.1
通讯作者：
Ye, Tao
中科院分区：
文献类型：
--
作者：
Cao, Huan H.;Abel, Gary R.;Gu, Qufei;Gueorguieva, Gloria-Alexandra V.;Zhang, Yehan;Nanney, Warren A.;Provencio, Eric T.;Ye, Tao
与超分子自组装方法不同，超分子自组装方法可以将许多不同的组件组织成均匀溶液中的设计形状（例如，DNA折纸），只有由几个不同组件组成的相对简单的对称结构才能在固体表面上自组装。由于自组装过程主要受非特异性吸引相互作用的限制，因此这些界面相互作用如何影响多组分自组装是一个悬而未决的问题。为了从机理上理解表面环境在DNA折纸自组装中的作用，我们研究了端系在动态表面上的长单链DNA （ssDNA支架）的寡核苷酸辅助折叠，该支架可以主动调节DNA -表面相互作用。结果表明，即使是微弱的表面引力也会通过抑制多畴合并成完整结构而导致缺陷结构。表面锚定和DNA -表面相互作用的刻意调节相结合，使我们能够通过非特异性相互作用脱离现有的表面限制范例，并使DNA折纸折叠在类似解决方案的环境中进行。重要的是，我们的策略保留了表面介导自组装的关键优势。例如，表面锚定的寡核苷酸可以序列特异性地启动特定大小和形状的DNA折纸的生长。我们的工作使信息能够被编码到一个表面，并表达成复杂的DNA表面结构，用于潜在的纳米电子和纳米光子应用。此外，我们的表面约束方法可以促进其他分子组分（如蛋白质）的二维自组装，因为保持构象自由可能是复杂结构在表面自组装的一个普遍挑战。
Unlike supramolecular self-assembly methods that can organize many distinct components into designer shapes in a homogeneous solution (e.g., DNA origami), only relatively simple, symmetric structures consisting of a few distinct components have been self-assembled at solid surfaces. As the self-assembly process is confined to the surface/interface by mostly nonspecific attractive interactions, an open question is how these interfacial interactions affect multicomponent self-assembly. To gain a mechanistic understanding of the roles of the surface environment in DNA origami self-assembly, here we studied the oligonucleotide-assisted folding of a long single-stranded DNA (ssDNA scaffold) that was end-tethered to a dynamic surface, which could actively regulate the DNA–surface interactions. The results showed that even weak surface attractions can lead to defective structures by inhibiting the merging of multiple domains into complete structures. A combination of surface anchoring and deliberate regulation of DNA–surface interactions allowed us to depart from the existing paradigm of surface confinement via nonspecific interactions and enabled DNA origami folding to proceed in a solution-like environment. Importantly, our strategy retains the key advantages of surface-mediated self-assembly. For example, surface-anchored oligonucleotides could sequence-specifically initiate the growth of DNA origamis of specific sizes and shapes. Our work enables information to be encoded into a surface and expressed into complex DNA surface architectures for potential nanoelectronic and nanophotonic applications. In addition, our approach to surface confinement may facilitate the 2D self-assembly of other molecular components, such as proteins, as maintaining conformational freedom may be a general challenge in the self-assembly of complex structures at surfaces.