Department of Chemical and Biomolecular Engineering, Johns Hopkins University, Baltimore, Maryland 21218, USA.
Department of Biomedical Engineering, Johns Hopkins University, Baltimore, Maryland 21218, USA.
Nanoscale. 2024 Jun 20;16(24):11688-11695. doi: 10.1039/d4nr01066c.
DNA nanotechnology offers many means to synthesize custom nanostructured materials from the ground up in a hierarchical fashion. While the assembly of DNA nanostructures from small (nanometer-scale) monomeric components has been studied extensively, how the hierarchical assembly of rigid or semi-flexible units produces multi-micron scale structures is less understood. Here we demonstrate a mechanism for assembling micron-scale semi-flexible DNA nanotubes into extended structures. These nanotubes assemble from nanometer-scale tile monomers into materials heterogeneous nucleation from rigid, Y-shaped DNA origami seeds to form Y-seeded nanotube architectures. These structures then assemble into networks nanotube end-to-end joining. We measure the kinetics of network growth and find that the assembly of networks can be approximated by a model of hierarchical assembly that assumes a single joining rate between DNA nanotube ends. Because the number of nucleation sites on Y-seeds and their spatial arrangement can be systematically varied by design, this hierarchical assembly process could be used to form a wide variety of networks and to understand the assembly mechanisms that lead to different types of material architectures at length scales of tens to hundreds of microns.
DNA 纳米技术提供了许多方法，可以从底层以分层的方式合成定制的纳米结构材料。虽然已经广泛研究了从小尺寸（纳米级）单体组件组装 DNA 纳米结构，但对于刚性或半刚性单元的层次组装如何产生多微米尺度结构的了解较少。在这里，我们展示了一种将微米级半刚性 DNA 纳米管组装成扩展结构的机制。这些纳米管由纳米级的瓦片单体组装而成，这些材料是从刚性的 Y 形 DNA 折纸种子异质成核形成 Y 形种子纳米管结构的。然后，这些结构组装成网络，通过纳米管末端的连接形成网络。我们测量了网络生长的动力学，并发现网络的组装可以通过一个假设 DNA 纳米管末端之间存在单一连接速率的层次组装模型来近似。由于 Y 形种子上的成核位点的数量及其空间排列可以通过设计进行系统地改变，因此这种层次组装过程可以用于形成各种网络，并了解导致不同类型材料结构的组装机制在数十到数百微米的长度尺度上。
