Pilyugina Ekaterina, Krajina Brad, Spakowitz Andrew J, Schieber Jay D
Center for Molecular Study of Condensed Soft Matter, Illinois Institute of Technology, Chicago, IL 60616, USA.
Department of Chemical and Biological Engineering, Illinois Institute of Technology, Chicago, IL 60616, USA.
Polymers (Basel). 2017 Mar 11;9(3):99. doi: 10.3390/polym9030099.
Instability and structural transitions arise in many important problems involving dynamics at molecular length scales. Buckling of an elastic rod under a compressive load offers a useful general picture of such a transition. However, the existing theoretical description of buckling is applicable in the load response of macroscopic structures, only when fluctuations can be neglected, whereas membranes, polymer brushes, filaments, and macromolecular chains undergo considerable Brownian fluctuations. We analyze here the buckling of a fluctuating semiflexible polymer experiencing a compressive load. Previous works rely on approximations to the polymer statistics, resulting in a range of predictions for the buckling transition that disagree on whether fluctuations elevate or depress the critical buckling force. In contrast, our theory exploits exact results for the statistical behavior of the worm-like chain model yielding unambiguous predictions about the buckling conditions and nature of the buckling transition. We find that a fluctuating polymer under compressive load requires a larger force to buckle than an elastic rod in the absence of fluctuations. The nature of the buckling transition exhibits a marked change from being distinctly second order in the absence of fluctuations to being a more gradual, compliant transition in the presence of fluctuations. We analyze the thermodynamic contributions throughout the buckling transition to demonstrate that the chain entropy favors the extended state over the buckled state, providing a thermodynamic justification of the elevated buckling force.
在许多涉及分子长度尺度动力学的重要问题中都会出现不稳定性和结构转变。弹性杆在压缩载荷下的屈曲为此类转变提供了一个有用的总体图景。然而,现有的屈曲理论仅在波动可忽略不计的情况下适用于宏观结构的载荷响应,而膜、聚合物刷、细丝和大分子链会经历相当大的布朗波动。我们在此分析承受压缩载荷的波动半柔性聚合物的屈曲。先前的工作依赖于聚合物统计的近似值,导致对于屈曲转变有一系列预测,这些预测在波动是提高还是降低临界屈曲力方面存在分歧。相比之下,我们的理论利用了蠕虫状链模型统计行为的精确结果,对屈曲条件和屈曲转变的性质给出了明确的预测。我们发现,承受压缩载荷的波动聚合物比无波动时的弹性杆需要更大的力才能屈曲。屈曲转变的性质呈现出明显变化,从无波动时明显的二级转变变为有波动时更渐进、更柔顺的转变。我们分析了整个屈曲转变过程中的热力学贡献,以证明链熵更倾向于伸展状态而非屈曲状态,从而为提高的屈曲力提供了热力学依据。