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拓扑缠结的自发打结聚电解质链通过纳米孔驱动。

Topological jamming of spontaneously knotted polyelectrolyte chains driven through a nanopore.

机构信息

SISSA-Scuola Internazionale Superiore di Studi Avanzati, Via Bonomea 265, 34136 Trieste, Italy.

出版信息

Phys Rev Lett. 2012 Sep 14;109(11):118301. doi: 10.1103/PhysRevLett.109.118301. Epub 2012 Sep 12.

Abstract

The advent of solid state nanodevices allows for interrogating the physicochemical properties of a polyelectrolyte chain by electrophoretically driving it through a nanopore. Salient dynamical aspects of the translocation process have been recently characterized by theoretical and computational studies of model polymer chains free from self-entanglement. However, sufficiently long equilibrated chains are necessarily knotted. The impact of such topological "defects" on the translocation process is largely unexplored, and is addressed in this Letter. By using Brownian dynamics simulations on a coarse-grained polyelectrolyte model we show that knots, despite being trapped at the pore entrance, do not per se cause the translocation process to jam. Rather, knots introduce an effective friction that increases with the applied force, and practically halts the translocation above a threshold force. The predicted dynamical crossover, which is experimentally verifiable, ought to be relevant in applicative contexts, such as DNA nanopore sequencing.

摘要

固态纳米器件的出现使得通过电泳将聚电解质链驱动通过纳米孔来检测其物理化学性质成为可能。最近,通过对无自缠结模型聚合物链的理论和计算研究,已经对易位过程的显著动态方面进行了表征。然而,足够长的平衡链必然是打结的。这种拓扑“缺陷”对易位过程的影响在很大程度上尚未得到探索,本研究信中对此进行了探讨。通过对粗粒化聚电解质模型进行布朗动力学模拟,我们表明,尽管结被捕获在孔口,但它们本身并不会导致易位过程发生堵塞。相反,结引入了一种与施加力成正比的有效摩擦力,并在超过阈值力时实际上会使易位过程停止。这种预测的动力学转变是可以在实验中验证的,应该与应用相关,例如 DNA 纳米孔测序。

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