解开生物聚合物溶液中的缠结
Disentangling Entanglements in Biopolymer Solutions
摘要：
爬行理论在解释缠结聚合物溶液的不寻常材料性质方面非常成功。它将复杂的多体动力学简化为单个聚合物的描述，其中每个聚合物被设想为被限制在一个管中，通过该管它以蛇形方式移动。对于柔性聚合物，爬行理论已经得到了实验和模拟的充分证实。与此相反，半柔性聚合物的实验和数值测试要么限于爬行的发病，或进行示踪聚合物在一个固定的，静态的矩阵。在这里，我们报告布朗动力学模拟的纠缠解决方案的半柔性聚合物，这表明，曲线运动沿管（爬行）不再是占主导地位的动力学模式。相反，我们发现，聚合物解开由于相关的约束释放，导致内部弯曲模式的平衡之前，聚合物扩散的整个管的长度。终端应力松弛的物理机制是旋转扩散介导的解开，而不是沿管的曲线运动。
英文摘要：
Reptation theory has been highly successful in explaining the unusual material properties of entangled polymer solutions. It reduces the complex many-body dynamics to a single-polymer description where each polymer is envisaged to be confined to a tube through which it moves in a snake-like fashion. For flexible polymers, reptation theory has been amply confirmed by both experiments and simulations. In contrast, for semiflexible polymers experimental and numerical tests are either limited to the onset of reptation, or were performed for tracer polymers in a fixed, static matrix. Here we report Brownian dynamics simulations of entangled solutions of semiflexible polymers, which show that curvilinear motion along a tube (reptation) is no longer the dominant mode of dynamics. Instead, we find that polymers disentangle due to correlated constraint release which leads to equilibration of internal bending modes before polymers diffuse the full tube length. The physical mechanism underlying terminal stress relaxation is rotational diffusion mediated by disentanglement rather than curvilinear motion along a tube.
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