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可寻址自组装中成核行为的直接观察和合理设计。

Direct observation and rational design of nucleation behavior in addressable self-assembly.

机构信息

Department of Diagnostics, Fraunhofer Institute for Cell Therapy and Immunology, 04103 Leipzig, Germany.

Faculty of Chemistry and Mineralogy, Leipzig University, 04103 Leipzig, Germany.

出版信息

Proc Natl Acad Sci U S A. 2018 Jun 26;115(26):E5877-E5886. doi: 10.1073/pnas.1806010115. Epub 2018 Jun 11.

DOI:10.1073/pnas.1806010115
PMID:29891671
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC6042111/
Abstract

To optimize a self-assembly reaction, it is essential to understand the factors that govern its pathway. Here, we examine the influence of nucleation pathways in a model system for addressable, multicomponent self-assembly based on a prototypical "DNA-brick" structure. By combining temperature-dependent dynamic light scattering and atomic force microscopy with coarse-grained simulations, we show how subtle changes in the nucleation pathway profoundly affect the yield of the correctly formed structures. In particular, we can increase the range of conditions over which self-assembly occurs by using stable multisubunit clusters that lower the nucleation barrier for assembling subunits in the interior of the structure. Consequently, modifying only a small portion of a structure is sufficient to optimize its assembly. Due to the generality of our coarse-grained model and the excellent agreement that we find with our experimental results, the design principles reported here are likely to apply generically to addressable, multicomponent self-assembly.

摘要

为了优化自组装反应，了解控制其途径的因素至关重要。在这里，我们研究了成核途径在基于典型“DNA 砖”结构的可寻址多组分自组装模型系统中的影响。通过将温度依赖性动态光散射和原子力显微镜与粗粒度模拟相结合，我们展示了成核途径的细微变化如何深刻影响正确形成结构的产率。特别是，我们可以通过使用稳定的多亚基簇来增加自组装发生的条件范围，这些亚基簇降低了在结构内部组装亚基的成核势垒。因此，只需修改结构的一小部分就足以优化其组装。由于我们的粗粒度模型具有普遍性，并且我们发现与实验结果非常吻合，因此这里报道的设计原则很可能普遍适用于可寻址的多组分自组装。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/e8c4/6042111/7a5a1d770ace/pnas.1806010115fig07.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/e8c4/6042111/bd5decae2dab/pnas.1806010115fig01.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/e8c4/6042111/2060b01e543d/pnas.1806010115fig02.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/e8c4/6042111/04d99606c494/pnas.1806010115fig03.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/e8c4/6042111/ad8ba102845c/pnas.1806010115fig04.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/e8c4/6042111/a5d3c399bbce/pnas.1806010115fig05.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/e8c4/6042111/13e726210a88/pnas.1806010115fig06.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/e8c4/6042111/7a5a1d770ace/pnas.1806010115fig07.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/e8c4/6042111/bd5decae2dab/pnas.1806010115fig01.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/e8c4/6042111/2060b01e543d/pnas.1806010115fig02.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/e8c4/6042111/04d99606c494/pnas.1806010115fig03.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/e8c4/6042111/ad8ba102845c/pnas.1806010115fig04.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/e8c4/6042111/a5d3c399bbce/pnas.1806010115fig05.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/e8c4/6042111/13e726210a88/pnas.1806010115fig06.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/e8c4/6042111/7a5a1d770ace/pnas.1806010115fig07.jpg

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