Piili J, Linna R P
Department of Computer Science, Aalto University, P.O. Box 15400, FI-00076 Aalto, Finland.
Phys Rev E Stat Nonlin Soft Matter Phys. 2015 Dec;92(6):062715. doi: 10.1103/PhysRevE.92.062715. Epub 2015 Dec 29.
We examine the ejection of an initially strongly confined flexible polymer from a spherical capsid through a nanoscale pore. We use molecular dynamics for unprecedentedly high initial monomer densities. We show that the time for an individual monomer to eject grows exponentially with the number of ejected monomers. By measurements of the force at the pore we show this dependence to be a consequence of the excess free energy of the polymer due to confinement growing exponentially with the number of monomers initially inside the capsid. This growth relates closely to the divergence of mixing energy in the Flory-Huggins theory at large concentration. We show that the pressure inside the capsid driving the ejection dominates the process that is characterized by the ejection time growing linearly with the lengths of different polymers. Waiting time profiles would indicate that the superlinear dependence obtained for polymers amenable to computer simulations results from a finite-size effect due to the final retraction of polymers' tails from capsids.
我们研究了一种最初被强烈限制在球形衣壳内的柔性聚合物通过纳米级孔隙的喷射过程。我们使用分子动力学方法来模拟前所未有的高初始单体密度情况。我们发现,单个单体喷射所需的时间随着喷射出的单体数量呈指数增长。通过测量孔隙处的力,我们表明这种依赖性是由于聚合物因限制而产生的过量自由能随着衣壳内初始单体数量呈指数增长所致。这种增长与弗洛里 - 哈金斯理论中在高浓度下混合能的发散密切相关。我们表明,驱动喷射的衣壳内压力主导了该过程,其特征是喷射时间与不同聚合物的长度呈线性增长。等待时间分布表明,对于适合计算机模拟的聚合物所获得的超线性依赖性是由于聚合物尾部从衣壳最终缩回导致的有限尺寸效应。