College of Engineering and Applied Sciences, State Key Laboratory of Analytical Chemistry for Life Science, National Laboratory of Solid State Microstructures, Jiangsu Key Laboratory of Artificial Functional Materials, Nanjing University, Nanjing, 210023, China.
Chemistry and Biomedicine Innovation Center, School of Chemistry and Chemical Engineering, Collaborative Innovation Center of Advanced Microstructures, Nanjing University, Nanjing, 210023, China.
J Am Chem Soc. 2020 Dec 23;142(51):21336-21343. doi: 10.1021/jacs.0c08525. Epub 2020 Dec 1.
Assembly of distinct types of species, particularly possessing anisotropic configurations, is the premise to broaden structural diversity and explore materials' collective properties. However, it remains a great challenge to programmably cocrystallize manifold anisotropic nanoparticles with the desired assembly mode, because it requires not only the complementarity of both sizes and shapes but also the control over their directional interactions. Here, by introducing DNA origami technique into lattice engineering, we synthesize two types of DNA nano-objects with different symmetries and program the heterogeneous functional patches precisely on their surfaces with nanometer-level precision, which could guide further assembly of these nano-objects. We show that these anisotropic DNA nano-objects could be cocrystallized along specified modes via modulating the combination of surface patches. The highly ordered DNA crystals were thoroughly evidenced by techniques including small-angle X-ray scattering and electron microscopy after careful encapsulation of a thin layer of silica on these DNA nano-objects. Our strategy endows distinct shapes of organic DNA origami structures with regulation features to control the sophisticated modes of cocrystallization of these diverse components, laying a foundation for designing and fabricating customized three-dimensional structures with given optical and mechanical properties.
不同类型物种的组装，特别是具有各向异性结构的物种组装，是拓宽结构多样性和探索材料集体性质的前提。然而，要以期望的组装模式可编程地共晶化多种各向异性纳米粒子仍然是一个巨大的挑战，因为它不仅需要大小和形状的互补性，还需要控制它们的方向相互作用。在这里，我们通过将 DNA 折纸技术引入到晶格工程中，合成了两种具有不同对称性的 DNA 纳米物体，并在其表面上以纳米级精度精确地编程了异质功能补丁，这可以指导这些纳米物体的进一步组装。我们表明，这些各向异性 DNA 纳米物体可以通过调节表面补丁的组合沿指定模式共晶化。在仔细地将一层薄的二氧化硅包裹在这些 DNA 纳米物体上之后，通过包括小角 X 射线散射和电子显微镜在内的技术，高度有序的 DNA 晶体得到了充分证实。我们的策略赋予了有机 DNA 折纸结构不同的形状调节特征，以控制这些不同组件的复杂共晶化模式，为设计和制造具有给定光学和机械性能的定制三维结构奠定了基础。
