SISSA, International School for Advanced Studies, via Bonomea 265, I-34136 Trieste, Italy.
SUPA, School of Physics, University of Edinburgh, Mayfield Road, Edinburgh EH9 3JZ, UK.
Nat Commun. 2015 Mar 10;6:6423. doi: 10.1038/ncomms7423.
The self-assembly of objects with a set of desired properties is a major goal of material science and physics. A particularly challenging problem is that of self-assembling structures with a target topology. Here we show by computer simulation that one may design the geometry of string-like rigid patchy templates to promote their efficient and reproducible self-assembly into a selected repertoire of non-planar closed folds including several knots. In particular, by controlling the template geometry, we can direct the assembly process so as to strongly favour the formation of constructs tied in trefoil or pentafoil, or even of more exotic torus knots. Polydisperse and racemic mixtures of helical fragments of variable composition add further tunability in the topological self-assembly we discovered. Our results should be relevant to the design of new ways to synthesize molecular knots, which may prove, for instance, to be efficient cargo-carriers due to their mechanical stability.
具有一组所需性质的物体的自组装是材料科学和物理学的主要目标。一个特别具有挑战性的问题是自组装具有目标拓扑的结构。在这里，我们通过计算机模拟表明，可以设计线状刚性有斑块模板的几何形状，以促进它们高效且可重复地自组装成包括几个结在内的非平面封闭折叠的选定曲目。特别是，通过控制模板几何形状，我们可以指导组装过程，从而强烈有利于三叶形或五叶形结，甚至是更奇特的环纽结的形成。具有可变组成的螺旋片段的多分散和外消旋混合物在我们发现的拓扑自组装中增加了进一步的可调性。我们的结果应该与设计新的合成分子结的方法有关，由于其机械稳定性，这些方法可能被证明是有效的货物载体。
