Physik Department, Walter Schottky Institute, Technische Universität München Am Coulombwall 4a, 85748 Garching near Munich, Germany.
Physik Department, Walter Schottky Institute, Technische Universität München Am Coulombwall 4a, 85748 Garching near Munich, Germany
Science. 2015 Mar 27;347(6229):1446-52. doi: 10.1126/science.aaa5372.
We demonstrate that discrete three-dimensional (3D) DNA components can specifically self-assemble in solution on the basis of shape-complementarity and without base pairing. Using this principle, we produced homo- and heteromultimeric objects, including micrometer-scale one- and two-stranded filaments and lattices, as well as reconfigurable devices, including an actuator, a switchable gear, an unfoldable nanobook, and a nanorobot. These multidomain assemblies were stabilized via short-ranged nucleobase stacking bonds that compete against electrostatic repulsion between the components' interfaces. Using imaging by electron microscopy, ensemble and single-molecule fluorescence resonance energy transfer spectroscopy, and electrophoretic mobility analysis, we show that the balance between attractive and repulsive interactions, and thus the conformation of the assemblies, may be finely controlled by global parameters such as cation concentration or temperature and by an allosteric mechanism based on strand-displacement reactions.
我们证明，离散的三维 (3D) DNA 组件可以基于形状互补性在溶液中特异性地自组装，而无需碱基配对。利用这一原理，我们制备了同型和异型多聚体物体，包括微米尺度的单链和双链纤维和晶格，以及可重构器件，包括执行器、可切换齿轮、可展开纳米书和纳米机器人。这些多结构域组装体通过短程核碱基堆积键稳定，这些键与组件界面之间的静电排斥作用相竞争。通过电子显微镜成像、集体和单分子荧光共振能量转移光谱以及电泳迁移率分析，我们表明，吸引力和排斥力之间的平衡，以及组装体的构象，可以通过全局参数（例如阳离子浓度或温度）和基于链置换反应的变构机制进行精细控制。
