Programming 2D Supramolecular Assemblies with Wireframe DNA Origami
Programming 2D Supramolecular Assemblies with Wireframe DNA Origami
复制标题
使用线框 DNA 折纸对 2D 超分子组装体进行编程
DOI：
10.1021/jacs.1c11332
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发表时间：
2022
影响因子：
15
通讯作者：
Bathe, Mark
中科院分区：
文献类型：
--
作者：
Wang, Xiao;Jun, Hyungmin;Bathe, Mark
线框DNA折纸提供了编程几乎任意的2D和3D纳米级几何形状的能力，具有六螺旋束（6HB）边缘设计，提供了相对于目标折纸形状的几何多功能性和保真度。由于单个DNA折纸对象的大小受到DNA支架长度的限制，在这里，我们引入了一种分层自组装策略，通过使用线框DNA折纸对象作为构建块编程超分子组装和周期阵列来克服这种限制。平行半交叉与斯台普斯和支架之间的横向内聚相互作用一起使用，以将对称性引入由单个DNA折纸单元构建的超分子组装体中，所述DNA折纸单元不能使用碱基堆积或常规反平行交叉设计直接自组装。这种分层设计方法可以很容易地应用于使用自顶向下的序列设计策略METIS设计的2D线框DNA折纸，而无需对支架和订书钉路由的任何先决条件。我们证明了我们的策略的效用，通过制造二聚体和自限制六聚体的上层结构，使用三角形和六边形的线框折纸积木。我们推广我们的自组装方法来制造紧密包装和非紧密包装的周期性二维阵列。使用原子力显微镜和透射电子显微镜的可视化表明，上层建筑表现出类似的结构完整性，使用METIS设计的个人折纸积木。我们的研究结果提供了一个通用的平台，为各种应用的二维材料的设计和制造。
Wireframe DNA origami offers the ability to program nearly arbitrary 2D and 3D nanoscale geometries, with six-helix bundle (6HB) edge designs providing both geometric versatility and fidelity with respect to the target origami shape. Because individual DNA origami objects are limited in size by the length of the DNA scaffold, here, we introduce a hierarchical self-assembly strategy to overcome this limitation by programming supramolecular assemblies and periodic arrays using wireframe DNA origami objects as building blocks. Parallel half-crossovers are used together with lateral cohesive interactions between staples and the scaffold to introduce symmetry into supramolecular assemblies constructed from single DNA origami units that cannot be self-assembled directly using base-stacking or conventional antiparallel crossover designs. This hierarchical design approach can be applied readily to 2D wireframe DNA origami designed using the top-down sequence design strategy METIS without any prerequisites on scaffold and staple routing. We demonstrate the utility of our strategy by fabricating dimers and self-limiting hexameric superstructures using both triangular and hexagonal wireframe origami building blocks. We generalize our self-assembly approach to fabricate close-packed and non-close-packed periodic 2D arrays. Visualization using atomic force microscopy and transmission electron microscopy demonstrates that superstructures exhibit similar structural integrity to that of the individual origami building blocks designed using METIS. Our results offer a general platform for the design and fabrication of 2D materials for a variety of applications.