Chemical Physics Department, Weizmann Institute of Science, Rehovot 7610001, Israel.
Soft Matter. 2017 Feb 7;13(5):995-1005. doi: 10.1039/c6sm02230h. Epub 2017 Jan 13.
Inhomogeneous polymers, such as partially cofilin-bound actin filaments, play an important role in various natural and biotechnological systems. At finite temperatures, inhomogeneous polymers exhibit non-trivial thermal fluctuations. More broadly, these are relatively simple examples of fluctuations in spatially inhomogeneous systems, which are less understood compared to their homogeneous counterparts. Here we develop a statistical theory of torsional, extensional and bending Gaussian fluctuations of inhomogeneous polymers (chains), where the inhomogeneity is an inclusion of variable size and stiffness, using both continuum and discrete approaches. First, we analytically calculate the complete eigenvalue and eigenmode spectra within a continuum field theory. In particular, we show that the wavenumber inside and outside of the inclusion is nearly linear in the eigenvalue index, with a nontrivial coefficient. Second, we solve the corresponding discrete problem and highlight fundamental differences between the continuum and discrete spectra. In particular, we demonstrate that above a certain wavenumber the discrete spectrum changes qualitatively and discrete evanescent eigenmodes, which do not have continuum counterparts, emerge. The implications of these differences are explored by calculating fluctuation-induced forces associated with free-energy variations with either the inclusion properties (e.g. inhomogeneity formed by adsorbing molecules) or with an external geometric constraint. The former, which is the fluctuation-induced contribution to the adsorbing molecule binding force, is shown to be affected by short wavelengths and thus cannot be calculated using the continuum approach. The latter, on the other hand, is shown to be dominated by long wavelength shape fluctuations and hence is properly described by the continuum theory.
不均匀聚合物,如部分与 cofilin 结合的肌动蛋白丝,在各种自然和生物技术系统中起着重要作用。在有限温度下,不均匀聚合物表现出非平凡的热涨落。更广泛地说,这些是空间不均匀系统涨落的相对简单的例子,与均匀系统相比,它们的理解程度较低。在这里,我们使用连续和离散方法,为不均匀聚合物(链)的扭转、拉伸和弯曲高斯涨落发展了一种统计理论,其中不均匀性是大小和刚度可变的包含物。首先,我们在连续场论中分析计算了完整的特征值和特征模谱。特别是,我们表明包含物内外的波数与特征值指数几乎呈线性关系,其中有一个非平凡的系数。其次,我们解决了相应的离散问题,并突出了连续谱和离散谱之间的基本区别。特别是,我们证明了在某个波数以上,离散谱会发生质的变化,并且会出现没有连续对应物的离散消逝本征模。通过计算与自由能变化相关的涨落诱导力来探索这些差异的影响,自由能变化与包含物性质(例如由吸附分子形成的不均匀性)或外部几何约束有关。前者是吸附分子结合力的涨落诱导贡献,它受到短波长的影响,因此不能使用连续体方法进行计算。另一方面,后者则被证明主要受到长波长形状波动的影响,因此可以用连续体理论正确描述。