Hydrodynamic interactions in topologically linked ring polymers
Hydrodynamic interactions in topologically linked ring polymers
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拓扑连接环聚合物中的流体动力学相互作用
DOI：
10.1103/physreve.102.032502
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发表时间：
2020
影响因子：
2.4
通讯作者：
de Pablo, Juan J.
中科院分区：
文献类型：
--
作者：
Rauscher, Phillip M.;Rowan, Stuart J.;de Pablo, Juan J.
尽管几十年来对拓扑连接的环聚合物进行了跨学科的研究，但它们的动力学在很大程度上仍然没有得到研究。这些系统是一个重大的科学挑战，因为它们经常受到拓扑和流体动力相互作用(HI)的影响，这使得动力学解要么在数学上难以处理，要么在计算上令人望而却步。在这里，我们通过预平均连接环的HI来绕过这些限制。我们发现，环聚合物的对称性导致了环动力学的流体动力解耦。即使对于非理想聚合物和非平衡条件，这种解偶联也是有效的。物理上，我们的发现表明，拓扑和HI的影响几乎是独立的，并不协同作用来影响聚合物的动力学。我们利用这一结果开发了比传统方法有巨大性能改进的高效布朗动力学算法，并应用这些算法模拟了平衡状态下的链状环状聚合物，证实了拓扑效应和HI的独立性。本文开发的方法可用于研究和模拟具有HI的大的环连接系统，包括动质DNA、奥林匹克凝胶和聚[]链烷。
Despite decades of interdisciplinary research on topologically linked ring polymers, their dynamics remain largely unstudied. These systems represent a major scientific challenge as they are often subject to both topological and hydrodynamic interactions (HI), which render dynamical solutions either mathematically intractable or computationally prohibitive. Here we circumvent these limitations by preaveraging the HI of linked rings. We show that the symmetry of ring polymers leads to a hydrodynamic decoupling of ring dynamics. This decoupling is valid even for nonideal polymers and nonequilibrium conditions. Physically, our findings suggest that the effects of topology and HI are nearly independent and do not act cooperatively to influence polymer dynamics. We use this result to develop highly efficient Brownian dynamics algorithms that offer enormous performance improvements over conventional methods and apply these algorithms to simulate catenated ring polymers at equilibrium, confirming the independence of topological effects and HI. The methods developed here can be used to study and simulate large systems of linked rings with HI, including kinetoplast DNA, Olympic gels, and poly[]catenanes.