发表机构
The University of Edinburgh; University of Padova（爱丁堡大学; 帕多瓦大学）
机构由 AI 辅助整理，请以论文原文为准。AI 中文总结
本研究通过分子动力学模拟，提出三种控制模式（缠结移动性、几何约束、动态重接线），将拓扑凝胶转化为可编程软材料，并揭示微观缠结动力学与宏观机械功能的设计原理。
AI 中文摘要
传统凝胶中的物理交联是静态且空间局域的，从根本上限制了其适应、自修复或执行机械功的能力。拓扑凝胶通过物理缠结（如穿线、链接和机械互锁）维系在一起，构成了另一种范式，即将连通性视为一种可移动的动态自由度。在此，我们通过半柔性聚合物和可穿线胶体环的分子动力学模拟，建立了一些通用的设计原理，将自组装拓扑凝胶转变为可编程软材料。我们提出了三种不同的控制模式。首先，通过控制缠结的移动性，可以调节材料的机械响应。淬火锚定迫使网络存储弹性应力并发生屈服，而退火锚定则使材料能够通过重新分布其缠结来松弛应力，同时保持全局连通性。其次，通过控制几何约束的程度或类型，可以模板化宏观结构，例如将三维各向同性凝胶转化为具有不同图谱谱特征的表面覆盖二维网络或准一维拓扑环。第三，通过允许通过聚合物重连进行缠结的动态重接线，可以在组装后重写材料拓扑，产生由简单成对链接主导的互锁结构，而非先前在重连柔性聚合物中观察到的高度复杂链接态。通过在微观缠结动力学与涌现的机械功能之间建立直接联系，我们的工作为自适应软超材料提供了设计原理，并为生物拓扑网络（如动质体DNA和染色质环网络）提供了见解。
英文摘要
Physical crosslinks in conventional gels are static and spatially localised, fundamentally limiting their capacity to adapt, self-heal, or perform mechanical work. Topological gels, which are held together by physical entanglements such as threadings, links, and mechanical interlocks, constitute a different paradigm by treating connectivity as a mobile, dynamic degree of freedom. Here, by using molecular dynamics simulations of semiflexible polymers and threadable colloidal rings, we establish some general design principles that transform self-assembled topological gels into programmable soft materials. We present three different modes of control. First, by controlling the mobility of the entanglements, one can tune the mechanical response of the material. Quenched anchoring forces the network to store elastic stress and yield, whereas with annealed anchoring the material can relax stresses by redistributing its entanglements whilst preserving global connectivity. Second, by controlling the degree or type of geometric confinement, it is possible to template macroscopic architecture, converting for instance 3D isotropic gels into surface-spanning 2D nets or quasi-1D topological rings with distinct graph-spectral signatures. Third, by allowing dynamical rewiring of entanglements through polymer reconnection, the material topology can be rewritten after assembly, yielding interlocked structures dominated by simple pairwise links rather than the highly complex linked states previously observed in reconnecting flexible polymers. By establishing a direct link between microscopic entanglement dynamics and emerging mechanical function, our work offers design principles for adaptive soft metamaterials and provides insights into biological topological networks such as kinetoplast DNA and chromatin loop networks.
