Through the strategic design of base sequences in DNA brushes, it is possible to adjust the interaction parameters between DNA-coated colloidal microspheres in tandem with their DNA grafting density and buffer conditions, resulting in a shift in their melting temperature. Multiple DNA-coated colloids can be assembled into hierarchical colloidal superstructures in a stepwise manner by tuning their respective melting temperatures. Here, the controlled introduction of mismatched base pairs into complementary DNA brushes provides an additional means of tuning the interparticle interactions. We find that precise control over the melting temperature can be achieved by strategically designing the type, position, or number of mismatched base pairs introduced in otherwise self-complementary DNA brushes. The use of two sets of particles coated with self-complementary DNA with dissimilar mismatched bases enables the realization of temperature-dependent binding with distinct melting temperatures. Using self-complementary DNA brushes with mismatched base pairs, two sets of colloidal particles are programmed with temperature-dependent orthogonal interactions to promote the stepwise assembly of the FCC-crystalline core–shell superstructures. Furthermore, to demonstrate the versatility of manipulating DNA sequences to engineer precise control over colloidal assembly, we demonstrate that CsCl-crystalline core–shell superstructures can be assembled from a ternary colloidal mixture by using complementary DNA brushes without or with mismatched bases.

中文翻译：

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用于逐步编程组装的具有碱基错配的 DNA 包被微球

通过对 DNA 刷中碱基序列的策略设计，可以根据 DNA 接枝密度和缓冲条件来调整 DNA 包被的胶体微球之间的相互作用参数，从而改变其熔解温度。通过调节各自的熔解温度，多种 DNA 包被的胶体可以逐步组装成分层的胶体超结构。在这里，将不匹配的碱基对受控地引入互补DNA刷中提供了调节颗粒间相互作用的另一种方法。我们发现，通过策略性地设计引入自互补DNA刷中的错配碱基对的类型、位置或数量，可以实现对解链温度的精确控制。使用两组涂有具有不同错配碱基的自互补 DNA 的颗粒，能够实现具有不同熔解温度的温度依赖性结合。使用具有不匹配碱基对的自互补 DNA 刷，两组胶体颗粒被编程为具有温度依赖性正交相互作用，以促进 FCC 晶体核壳超结构的逐步组装。此外，为了证明操纵DNA序列以设计对胶体组装的精确控制的多功能性，我们证明了CsCl结晶核壳超结构可以通过使用不带或不带错配碱基的互补DNA刷从三元胶体混合物组装而成。