Physics Department, Technical University Munich, 85748 Garching, Germany.
J Chem Phys. 2011 Jun 21;134(23):235102. doi: 10.1063/1.3593458.
The influence of hydrodynamic screening near a surface on the dynamics of a single semiflexible polymer is studied by means of Brownian dynamics simulations and hydrodynamic mean field theory. The polymer motion is characterized in terms of the mean squared displacements of the end-monomers, the end-to-end vector, and the scalar end-to-end distance. In order to control hydrodynamic screening effects, the polymer is confined to a plane at a fixed separation from the wall. When gradually decreasing this separation, a crossover from Zimm-type towards Rouse (free-draining) polymer dynamics is induced. However, this crossover is rather slow and the free-draining limit is not completely reached--substantial deviations from Rouse-like dynamics are registered in both simulations and theory--even at distances of the polymer from the wall on the order of the monomer size. Remarkably, the effect of surface-induced screening of hydrodynamic interactions sensitively depends on the type of dynamic observable considered. For vectorial quantities such as the end-to-end vector, hydrodynamic interactions are important and therefore surface screening effects are sizeable. For a scalar quantity such as the end-to-end distance, on the other hand, hydrodynamic interactions are less important, but a pronounced dependence of dynamic scaling exponents on the persistence length to contour length ratio becomes noticeable. Our findings are discussed against the background of single-molecule experiments on f-actin [L. Le Goff et al., Phys. Rev. Lett. 89, 258101 (2002)].
通过布朗动力学模拟和流体力学平均场理论研究了表面附近流体动力屏蔽对单根半柔性聚合物动力学的影响。通过末端单体的均方位移、末端到末端向量和标量末端到末端距离来描述聚合物的运动。为了控制流体动力屏蔽效应,将聚合物限制在与壁面固定分离的平面内。当逐渐减小这种分离时,从 Zimm 型到 Rouse(自由排水)聚合物动力学的转变会被诱导。然而,这种转变相当缓慢,并且即使在聚合物与壁面的距离为单体尺寸量级时,也无法完全达到自由排水的极限——在模拟和理论中都记录到与 Rouse 型动力学有很大偏差。值得注意的是,表面诱导的流体动力相互作用的屏蔽效应强烈依赖于所考虑的动态观测量的类型。对于末端到末端向量等向量量,流体动力相互作用很重要,因此表面屏蔽效应相当大。另一方面,对于末端到末端距离等标量量,流体动力相互作用不太重要,但动态标度指数对持久长度与轮廓长度比的明显依赖性变得明显。我们的发现是在单分子实验的背景下讨论的,实验对象是 f-肌动蛋白[L. Le Goff 等人,Phys. Rev. Lett. 89, 258101 (2002)]。