Trapped entanglements─topological cross-links among polymer chains in a network─are fundamental to polymers and have been correlated with mechanical properties like toughness, critical for virtually any application of soft materials. Yet, although the concept of polymer entanglement has been around over 80 years, entanglement topology–property relationships remain ill-defined because we lack methods to experimentally install and quantify entanglements with precise topologies. Here, we use supramolecular templates based on phenanthroline-copper(I) complexes to install into poly(methoxyethyl acrylate) elastomer-trapped entanglements whose topology is programmed by the complex geometry. Compared to control materials, we observe 17% diminished swelling and 29% enhanced modulus, with only 0.75 mol % of the entanglement template or 1.5 mol % of the ligand. Moreover, we discovered that fluorescent phenanthroline-based exciplexes formed selectively when entanglement-templating complexes were used, which could in the future enable detection and direct quantification of supramolecular templated entanglements.

中文翻译：

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聚合物弹性体中缠结的超分子模板及其光谱检测

捕获缠结（网络中聚合物链之间的拓扑交联）是聚合物的基础，并且与韧性等机械性能相关，这对于软材料的几乎所有应用都至关重要。然而，尽管聚合物缠结的概念已经存在了 80 多年，但缠结拓扑-性质关系仍然不明确，因为我们缺乏通过实验安装和量化具有精确拓扑的缠结的方法。在这里，我们使用基于菲咯啉-铜（I）络合物的超分子模板将其安装到聚（丙烯酸甲氧基乙酯）弹性体捕获的缠结中，其拓扑结构由复杂的几何形状编程。与对照材料相比，我们观察到溶胀减少了 17%，模量增加了 29%，仅使用 0.75 mol% 的缠结模板或 1.5 mol% 的配体。此外，我们发现，当使用纠缠模板复合物时，基于荧光菲咯啉的激基复合物会选择性形成，这在未来可以实现超分子模板纠缠的检测和直接定量。