PolyA-based DNA bonds with programmable bond length and bond energy
PolyA-based DNA bonds with programmable bond length and bond energy
复制标题
具有可编程键长和键能的基于 PolyA 的 DNA 键
DOI：
10.1038/s41427-020-0231-x
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发表时间：
2020-07-03
影响因子：
9.7
通讯作者：
Li, Jiang
中科院分区：
文献类型：
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作者：
Chen, Xiaoliang;Liu, Xiaoguo;Li, Jiang
DNA功能化的金纳米颗粒(AuNPs)作为可编程原子当量(PAE)被广泛应用于类分子结构的自组装。然而，通过不同水平的离散DNA键构建层次化的PAE组装仍然具有挑战性。在这里，我们报告了一种策略，使用携带连续腺嘌呤(PolyA)的DNA编码器来编程PAE上的DNA键长和键能。在AuNPs上，我们构建了三种不同拓扑结构的DNA基序，它们可以形成PAE自组装的键。通过小角X射线散射(SAXS)分析，我们发现可以通过对键结构的编程来调节偶联PAE之间的键长和柔性。我们还发现，这些键显示不同的键能，因此根据它们的拓扑结构而不同，从而导致不同的PAE组装效率。我们证明了不同水平的键可以在一个纳米颗粒上以不同的方向排列，从而导致不对称的PAE，允许多粒子结构的离子强度控制的分级组装。这种可编程键合系统可能为构建复杂的等离子体超结构提供一条新的途径。
DNA-functionalized Au nanoparticles (AuNPs) have been intensively exploited as programmable atom equivalents (PAEs) for the self-assembly of molecule-like structures. However, it remains challenging to build hierarchical PAE assemblies via discrete DNA bonds at different levels. Here, we report a strategy to program DNA bond length and bond energy on PAEs using DNA encoders carrying consecutive adenines (polyA). On AuNPs, we built three types of DNA motifs with different topologic configurations, which can form bonds for PAE self-assembly. By small-angle X-ray scattering (SAXS) analysis, we found that the bond length and flexibility between the coupled PAEs can be tuned by programming the bond structure. We also found that these bonds show different bond energies and thus differ, depending on their topologic configuration, leading to different PAE assembly efficiencies. We demonstrated that the bonds at different levels can be arranged in different directions on one nanoparticle, leading to asymmetric PAEs that allow ionic strength-controlled hierarchical assembly of multiparticle structures. This programmable bonding system may provide a new route for building complex plasmonic superstructures.