Reversible Polymerization-like Kinetics for Programmable Self-Assembly of DNA-Encoded Nanoparticles with Limited Valence
Reversible Polymerization-like Kinetics for Programmable Self-Assembly of DNA-Encoded Nanoparticles with Limited Valence
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有限价 DNA 编码纳米颗粒可编程自组装的可逆类聚合动力学
DOI：
10.1021/jacs.9b07919
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发表时间：
2019-10-16
影响因子：
15
通讯作者：
Lin, Jiaping
中科院分区：
文献类型：
--
作者：
Gu, Mengxin;Ma, Xiaodong;Lin, Jiaping
分子的聚合反应和纳米粒子的自组装之间的相似性为可靠地预测纳米粒子集合的结构特征提供了一种独特的方法。然而，由于DNA链的杂交和去杂交的存在，对DNA编码纳米颗粒的可编程自组装动力学的定量阐明仍然是具有挑战性的。本文发展了一种理论与计算相结合的方法来解释表面编码互补DNA链的有限价态纳米粒子可编程自组装的机理和动力学。结果表明，DNA编码的纳米颗粒被编程以形成一系列具有复杂结构的自组装超结构，如线性链、溶胶和纳米颗粒的凝胶。理论上证明了有限价态DNA编码纳米粒子的可编程自组装一般遵循最初在聚合物科学中提出的可逆步长聚合的动力学和统计规律。此外，应用理论计算方法捕捉了二价DNA-蛋白质偶联物的可编程自组装行为。所获得的结果不仅为DNA编码纳米颗粒的可编程自组装提供了基本的见解，也为具有复杂结构的DNA编程超结构提供了设计规则。
A similarity between the polymerization reaction of molecules and the self-assembly of nanoparticles provides a unique way to reliably predict structural characteristics of nanoparticle ensembles. However, the quantitative elucidation of programmable self-assembly kinetics of DNA-encoded nanoparticles is still challenging due to the existence of hybridization and dehybridization of DNA strands. Herein, a joint theoretical-computational method is developed to explicate the mechanism and kinetics of programmable self-assembly of limited-valence nanoparticles with surface encoding of complementary DNA strands. It is revealed that the DNA-encoded nanoparticles are programmed to form a diverse range of self-assembled superstructures with complex architecture, such as linear chains, sols, and gels of nanoparticles. It is theoretically demonstrated that the programmable self-assembly of DNA-encoded nanoparticles with limited valence generally obeys the kinetics and statistics of reversible step-growth polymerization originally proposed in polymer science. Furthermore, the theoretical-computational method is applied to capture the programmable self-assembly behavior of bivalent DNA-protein conjugates. The obtained results not only provide fundamental insights into the programmable self-assembly of DNA-encoded nanoparticles but also offer design rules for the DNA-programmed superstructures with elaborate architecture.