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具有主动噪声的半柔性聚合物的内部动力学。

Internal dynamics of semiflexible polymers with active noise.

机构信息

Theoretical Soft Matter and Biophysics, Institute of Complex Systems and Institute for Advanced Simulation, Forschungszentrum Jülich, D-52425 Jülich, Germany.

出版信息

J Chem Phys. 2017 Apr 21;146(15):154903. doi: 10.1063/1.4981012.

Abstract

The intramolecular dynamics of flexible and semiflexible polymers in response to active noise is studied theoretically. The active noise may either originate from interactions of a passive polymer with a bath of active Brownian particles or the polymer itself is comprised of active Brownian particles. We describe the polymer by the continuous Gaussian semiflexible-polymer model, taking into account the finite polymer extensibility. Our analytical calculations predict a strong dependence of the polymer dynamics on the activity. In particular, active semiflexible polymers exhibit a crossover from a bending elasticity-dominated dynamics at weak activity to that of flexible polymers at strong activity. The end-to-end vector correlation function decays exponentially for times longer than the longest polymer relaxation time. Thereby, the polymer relaxation determines the decay of the correlation function for long and flexible polymers. For shorter and stiffer polymers, the relaxation behavior of individual active Brownian particles dominates the decay above a certain activity. The diffusive dynamics of a polymer is substantially enhanced by the activity. Three regimes can be identified in the mean square displacement for sufficiently strong activities: an activity-induced ballistic regime at short times, followed by a Rouse-type polymer-specific regime for any polymer stiffness, and free diffusion at long times, again determined by the activity.

摘要

理论研究了柔性和半柔性聚合物对活性噪声的分子内动力学。活性噪声可能源自于被动聚合物与活性布朗粒子浴的相互作用,或者聚合物本身由活性布朗粒子组成。我们通过连续高斯半柔性聚合物模型来描述聚合物,考虑到聚合物的有限延伸性。我们的分析计算预测了聚合物动力学对活性的强烈依赖性。具体而言,活性半柔性聚合物在弱活性下表现出弯曲弹性主导的动力学,而在强活性下表现出柔性聚合物的动力学。对于时间长于最长聚合物弛豫时间的情况,末端向量相关函数呈指数衰减。因此,对于长而柔性的聚合物,聚合物弛豫决定了相关函数的衰减。对于更短和更硬的聚合物,在一定活性以上,单个活性布朗粒子的弛豫行为主导着衰减。活性大大增强了聚合物的扩散动力学。对于足够强的活性,可以在平均平方位移中识别出三个区域:短时间内的活性诱导弹道区域,随后是任何聚合物刚度的罗瑟型聚合物特有的区域,以及长时间内的自由扩散,再次由活性决定。

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