Self-assembly of emulsion droplets through programmable folding
Self-assembly of emulsion droplets through programmable folding
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DOI：
10.1038/s41586-022-05198-8
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发表时间：
2022-09-28
期刊：
影响因子：
64.8
通讯作者：
Brujic, Jasna
中科院分区：
文献类型：
--
作者：
McMullen, Angus;Basagoiti, Maitane Munoz;Brujic, Jasna
在粒子自组装领域，如果所有的碎片都是不同的，就有可能可靠地构建几乎任意的结构（1-3），但是到目前为止，具有较少构建块味道的系统仅限于奇异晶体的组装（4-6）。在这里，我们介绍了一个胶体液滴链的最小模型系统（7），具有可编程的DNA相互作用，引导它们向下折叠成特定的几何形状。水滴在真实的空间和时间中被观察到，解开了折叠的规则。结合实验，模拟和理论，我们表明，控制相互作用打开的顺序可以指导折叠成独特的结构，我们称之为胶体折叠体（8）。最简单的交替序列（ABAB...）最多13个液滴产生11个二维折叠体和一个三维折叠体。优化液滴序列并添加额外的风味独特地编码了619种可能的二维几何形状中的一半以上。由至少13个液滴组成的折叠体呈现具有孔的开放结构，提供多孔设计。数值模拟表明，折叠体可以进一步相互作用，使复杂的超胶体结构，如二聚体，带状和马赛克。我们的研究结果是独立的动力学，因此适用于聚合物材料的所有长度尺度上的层次相互作用，从有机分子的所有方式魔方的蛇。这个工具箱能够将大规模设计编码成短聚合物序列，将折叠置于材料自组装的最前沿。
In the realm of particle self-assembly, it is possible to reliably construct nearly arbitrary structures if all the pieces are distinct(1-3), but systems with fewer flavours of building blocks have so far been limited to the assembly of exotic crystals(4-6). Here we introduce a minimal model system of colloidal droplet chains(7), with programmable DNA interactions that guide their downhill folding into specific geometries. Droplets are observed in real space and time, unravelling the rules of folding. Combining experiments, simulations and theory, we show that controlling the order in which interactions are switched on directs folding into unique structures, which we call colloidal foldamers(8). The simplest alternating sequences (ABAB...) of up to 13 droplets yield 11 foldamers in two dimensions and one in three dimensions. Optimizing the droplet sequence and adding an extra flavour uniquely encodes more than half of the 619 possible two-dimensional geometries. Foldamers consisting of at least 13 droplets exhibit open structures with holes, offering porous design. Numerical simulations show that foldamers can further interact to make complex supracolloidal architectures, such as dimers, ribbons and mosaics. Our results are independent of the dynamics and therefore apply to polymeric materials with hierarchical interactions on all length scales, from organic molecules all the way to Rubik's Snakes. This toolbox enables the encoding of large-scale design into sequences of short polymers, placing folding at the forefront of materials self-assembly.