Tsang Boyce, Dell Zachary E, Jiang Lingxiang, Schweizer Kenneth S, Granick Steve
Department of Physics, University of Illinois at Urbana-Champaign, Urbana, IL 61801.
Department of Materials Science and Engineering, Jinan University, Guangzhou 510632, China.
Proc Natl Acad Sci U S A. 2017 Mar 28;114(13):3322-3327. doi: 10.1073/pnas.1620935114. Epub 2017 Mar 10.
Entanglement in polymer and biological physics involves a state in which linear interthreaded macromolecules in isotropic liquids diffuse in a spatially anisotropic manner beyond a characteristic mesoscopic time and length scale (tube diameter). The physical reason is that linear macromolecules become transiently localized in directions transverse to their backbone but diffuse with relative ease parallel to it. Within the resulting broad spectrum of relaxation times there is an extended period before the longest relaxation time when filaments occupy a time-averaged cylindrical space of near-constant density. Here we show its implication with experiments based on fluorescence tracking of dilutely labeled macromolecules. The entangled pairs of aqueous F-actin biofilaments diffuse with separation-dependent dynamic cross-correlations that exceed those expected from continuum hydrodynamics up to strikingly large spatial distances of ≈15 µm, which is more than 10 times the size of the solvent water molecules in which they are dissolved, and is more than 50 times the dynamic tube diameter, but is almost equal to the filament length. Modeling this entangled system as a collection of rigid rods, we present a statistical mechanical theory that predicts these long-range dynamic correlations as an emergent consequence of an effective long-range interpolymer repulsion due to the de Gennes correlation hole, which is a combined consequence of chain connectivity and uncrossability. The key physical assumption needed to make theory and experiment agree is that solutions of entangled biofilaments localized in tubes that are effectively dynamically incompressible over the relevant intermediate time and length scales.
聚合物与生物物理学中的缠结涉及一种状态,即各向同性液体中的线性相互交织的大分子在超过特征介观时间和长度尺度(管径)后以空间各向异性的方式扩散。物理原因是线性大分子在垂直于其主链的方向上暂时定位,但沿主链方向相对容易扩散。在由此产生的宽弛豫时间谱中,在最长弛豫时间之前有一个扩展期,此时细丝占据密度近似恒定的时间平均圆柱形空间。在此,我们通过基于对稀释标记大分子的荧光追踪的实验展示其意义。成对缠结的水性F-肌动蛋白生物丝以与分离相关的动态互相关进行扩散,这种互相关超过了连续介质流体动力学预期的值,直至惊人的大空间距离≈15µm,这是其溶解的溶剂水分子大小的10倍以上,是动态管径的50倍以上,但几乎等于细丝长度。将这个缠结系统建模为一组刚性棒,我们提出了一种统计力学理论,该理论预测这些长程动态相关性是由于德热纳关联空穴导致的有效长程聚合物间排斥的一种涌现结果,德热纳关联空穴是链连接性和不可穿越性的综合结果。使理论与实验相符所需的关键物理假设是,缠结生物丝的溶液在相关的中间时间和长度尺度上有效地动态不可压缩,且局限于管中。