Xia Xiuyang, Hu Hao, Ciamarra Massimo Pica, Ni Ran
Chemical Engineering, School of Chemical and Biomedical Engineering, Nanyang Technological University, 62 Nanyang Drive, Singapore 637459.
Division of Physics and Applied Physics, School of Physical and Mathematical Sciences, Nanyang Technological University, 21 Nanyang Link, Singapore 637371.
Sci Adv. 2020 May 20;6(21):eaaz6921. doi: 10.1126/sciadv.aaz6921. eCollection 2020 May.
Developing construction methods of materials tailored for given applications with absolute control over building block placement poses an immense challenge. DNA-coated colloids offer the possibility of realising programmable self-assembly, which, in principle, can assemble almost any structure in equilibrium, but remains challenging experimentally. Here, we propose an innovative system of linker-mediated mobile DNA-coated colloids (mDNACCs), in which mDNACCs are bridged by the free DNA linkers in solution, whose two single-stranded DNA tails can bind with specific single-stranded DNA receptors of complementary sequence coated on colloids. We formulate a mean-field theory efficiently calculating the effective interaction between mDNACCs, where the entropy of DNA linkers plays a nontrivial role. Particularly, when the binding between free DNA linkers in solution and the corresponding receptors on mDNACCs is strong, the linker-mediated colloidal interaction is determined by the linker entropy depending on the linker concentration.
开发针对特定应用量身定制的材料构建方法，并对构建块的放置进行绝对控制，这是一项巨大的挑战。DNA包覆的胶体提供了实现可编程自组装的可能性，原则上，它可以在平衡状态下组装几乎任何结构，但在实验上仍然具有挑战性。在这里，我们提出了一种创新的连接子介导的移动DNA包覆胶体（mDNACC）系统，其中mDNACC通过溶液中的游离DNA连接子桥接，其两条单链DNA尾巴可以与包覆在胶体上的互补序列的特定单链DNA受体结合。我们制定了一种平均场理论，有效地计算mDNACC之间的有效相互作用，其中DNA连接子的熵起着重要作用。特别是，当溶液中的游离DNA连接子与mDNACC上的相应受体之间的结合很强时，连接子介导的胶体相互作用由取决于连接子浓度的连接子熵决定。
