End-Monomer Dynamics in Semiflexible Polymers

被引:36
作者
Hinczewski, Michael [1 ]
Schlagberger, Xaver [2 ]
Rubinstein, Michael [3 ]
Krichevsky, Oleg [4 ]
Netz, Roland R. [2 ]
机构
[1] Bosphorus Univ, TUBITAK, Feza Gursey Res Inst, TR-34684 Istanbul, Turkey
[2] Tech Univ Munich, Dept Phys, D-85748 Garching, Germany
[3] Univ N Carolina, Dept Chem, Chapel Hill, NC 27599 USA
[4] Ben Gurion Univ Negev, Dept Phys, IL-84105 Beer Sheva, Israel
基金
美国国家科学基金会;
关键词
SCATTERING; DIFFUSION; VISCOELASTICITY; MACROMOLECULES; MICRORHEOLOGY; MODEL;
D O I
10.1021/ma802017g
中图分类号
O63 [高分子化学(高聚物)];
学科分类号
070305 ; 080501 ; 081704 ;
摘要
Spurred by an experimental controversy in the literature, we investigate the end-monomer dynamics of semiflexible polymers through Brownian hydrodynamic simulations and dynamic mean-field theory. Precise experimental observations over the past few years of end-monomer dynamics in the diffusion of double-stranded DNA have given conflicting results: one study indicated an unexpected Rouse-like scaling of the mean-squared displacement (MSD) < r(2)(t)> similar to t(1/2) at intermediate times, corresponding to fluctuations at length scales larger than the persistence length but smaller than the coil size; another study claimed the more conventional Zimm scaling < r(2)(t)> similar to t(2/3) in the same time range. Using hydrodynamic simulations as well as analytical and scaling theories, we find a novel intermediate dynamical regime where the effective local exponent of the end-monomer MSD, alpha(t) = d(log < r(2)(t)>)/d(log t) drops below the Zimm value of 2/3 for sufficiently long chains. The deviation from the Zimm prediction increases with chain length, though it does not reach the Rouse limit of 1/2. The qualitative features of this intermediate regime, found in simulations and in an improved mean-field theory for semiflexible polymers, in particular the variation of alpha(t) with chain and persistence lengths, can be reproduced through a heuristic scaling argument. Anomalously low values of the effective exponent a are explained by hydrodynamic effects related to the slow crossover from dynamics on length scales smaller than the persistence length to dynamics on larger length scales.
引用
收藏
页码:860 / 875
页数:16
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