Novak Sanja, Zhang Jing, Kentzinger Emmanuel, Rücker Ulrich, Portale Giuseppe, Jung Niklas, Jonas Ulrich, Myung Jin S, Winkler Roland G, Gompper Gerhard, Dhont Jan K G, Stiakakis Emmanuel
Biomacromolecular Systems and Processes, Institute of Biological Information Processing (IBI-4), Forschungszentrum Jülich, D-52425 Jülich, Germany.
Jülich Centre for Neutron Science JCNS and Peter Grünberg Institut PGI, JARA-FIT, Forschungszentrum Jülich, D-52425 Jülich, Germany.
ACS Nano. 2020 Oct 27;14(10):13524-13535. doi: 10.1021/acsnano.0c05536. Epub 2020 Oct 13.
Adding shape and interaction anisotropy to a colloidal particle offers exquisitely tunable routes to engineer a rich assortment of complex-architected structures. Inspired by the hierarchical self-assembly concept with block copolymers and DNA liquid crystals and exploiting the unique assembly properties of DNA, we report here the construction and self-assembly of DNA-based soft-patchy anisotropic particles with a high degree of modularity in the system's design. By programmable positioning of thermoresponsive polymeric patches on the backbone of a stiff DNA duplex with linear and star-shaped architecture, we reversibly drive the DNA from a disordered ensemble to a diverse array of long-range ordered multidimensional nanostructures with tunable lattice spacing, ranging from lamellar to bicontinuous double-gyroid and double-diamond cubic morphologies, through the alteration of temperature. Our results demonstrate that the proposed hierarchical self-assembly strategy can be applied to any kind of DNA nanoarchitecture, highlighting the design principles for integration of self-assembly concepts from the physics of liquid crystals, block copolymers, and patchy colloids into the continuously growing interdisciplinary research field of structural DNA nanotechnology.
给胶体粒子添加形状和相互作用各向异性，为构建种类丰富的复杂结构提供了极为可调的途径。受嵌段共聚物和DNA液晶的分级自组装概念启发，并利用DNA独特的组装特性，我们在此报告了基于DNA的软斑状各向异性粒子的构建与自组装，该粒子在系统设计中具有高度模块化。通过将热响应性聚合物补丁可编程地定位在具有线性和星形结构的刚性DNA双链体主链上，我们通过改变温度，可逆地将DNA从无序聚集体驱动到一系列具有可调晶格间距的长程有序多维纳米结构，其形态从层状到双连续双螺旋面和双菱形立方形态不等。我们的结果表明，所提出的分级自组装策略可应用于任何种类的DNA纳米结构，突出了将液晶、嵌段共聚物和斑状胶体物理学中的自组装概念整合到不断发展的结构DNA纳米技术跨学科研究领域的设计原则。
