Hsiao Pai-Yi
Department of Engineering and System Science, National Tsing Hua University, Hsinchu, Taiwan 30013, R. O. C.
Institute of Nuclear Engineering and Science, National Tsing Hua University, Hsinchu, Taiwan 30013, R. O. C.
ACS Omega. 2020 Jul 22;5(31):19805-19819. doi: 10.1021/acsomega.0c02647. eCollection 2020 Aug 11.
A polyelectrolyte threading through a nanopore in a trivalent salt solution is investigated by means of molecular dynamics simulations under a reflective wall boundary. By varying the chain length and the strength of the driving electric field applied inside the pore, the translocation time is carefully calculated to get rid of the bouncing effect because of the boundary. The results are analyzed under the scaling form ⟨τ⟩ ∼ and four driving force regimes; namely, the unbiased, the weakly driven, the strongly driven trumpet, and the strongly driven isoflux regime, are distinguished. The exponents are calculated in each regime and compared with the cases in the monovalent and divalent salt solutions. Owing to strong condensation of counter ions, the changes of the exponents in the force regimes are found to be nontrivial. A large increase in translocation time can be, however, achieved as the driving field is weak. The variations of the chain size, the ion condensation, and the effective chain charge show that the process is proceeded in a quasi-equilibrium way in the unbiased regime and deviated to exhibit strong nonequilibrium characteristics as increases. Several astonishing scaling behaviors of the waiting time function, the translocation velocity, and the diffusion properties are discovered in the study. The results provide deep insights into the phenomena of polyelectrolyte translocation in various salt solutions at different driving forces.
通过分子动力学模拟,在反射壁边界条件下研究了在三价盐溶液中穿过纳米孔的聚电解质。通过改变链长和施加在孔内的驱动电场强度,仔细计算了转运时间以消除由于边界引起的反弹效应。结果以标度形式⟨τ⟩ ∼ 进行分析,并区分了四种驱动力 regime;即无偏、弱驱动、强驱动喇叭形和强驱动等通量 regime。计算了每个 regime 中的指数,并与单价和二价盐溶液中的情况进行了比较。由于反离子的强烈凝聚,发现力 regime 中指数的变化是不平凡的。然而,当驱动场较弱时,可以实现转运时间的大幅增加。链尺寸、离子凝聚和有效链电荷的变化表明,该过程在无偏 regime 中以准平衡方式进行,并且随着 的增加偏离以表现出强非平衡特征。在研究中发现了等待时间函数、转运速度和扩散性质的几种惊人的标度行为。这些结果为不同驱动力下各种盐溶液中聚电解质转运现象提供了深刻见解。