Polles Guido, Orlandini Enzo, Micheletti Cristian
SISSA, International School for Advanced Studies, via Bonomea 265, I-34136 Trieste, Italy.
Dipartimento di Fisica e Astronomia and Sezione INFN, Universita' di Padova, Via Marzolo 8, 35131 Padova, Italy.
ACS Macro Lett. 2016 Aug 16;5(8):931-935. doi: 10.1021/acsmacrolett.6b00425. Epub 2016 Jul 18.
How to direct the self-assembly of simple templates toward constructs with complex shape and topology is still an open problem. Recent advancements have made it possible to self-assemble various types of knotted constructs, but targeting general multicomponent topologies, that is, links and catenanes, has proved much harder. Here, we study how the yield and complexity of self-assembled links depends on both intrinsic and extrinsic system properties and, particularly, template shape and spatial confinement. We show that slit confinement does not necessarily suppress linking but can rather enhance it significantly thanks to entropic effects. We also found that only a limited set of binary links are recurrent for different template shapes. These privileged topologies include all those experimentally realized so far plus a few additional ones, such as the 7 and 7 links that, hence, ought to be ideal candidates for broadening the current class of constructs with addressable topology.
如何将简单模板的自组装导向具有复杂形状和拓扑结构的构建体仍是一个悬而未决的问题。最近的进展使得自组装各种类型的打结构建体成为可能，但针对一般的多组分拓扑结构，即链环和索烃，已证明要困难得多。在这里，我们研究自组装链环的产率和复杂性如何取决于内在和外在的系统特性，特别是模板形状和空间限制。我们表明，狭缝限制不一定会抑制连接，相反，由于熵效应，它反而可以显著增强连接。我们还发现，对于不同的模板形状，只有有限的一组二元链环是重复出现的。这些特殊的拓扑结构包括迄今为止所有通过实验实现的结构，以及一些额外的结构，例如7₁和7₂链环，因此，它们应该是拓宽当前具有可寻址拓扑结构的构建体类别的理想候选者。
