发表机构
Indian Institute of Technology Jodhpur; University of Delhi（印度理工学院乔德普尔分校; 德里大学）
机构由 AI 辅助整理，请以论文原文为准。AI 中文总结
本研究通过混合CR蒙特卡罗/分子动力学模拟，探究电荷调控对聚电解质吸附带相反电荷纳米粒子的构象与动力学影响，发现高盐下CR增强吸附、CC促伸展构象等规律，为调控纳米粒子稳定性提供策略。
AI 中文摘要
利用聚电解质定制纳米粒子的表面特性与刺激响应行为，正开启从高级诊断到实际应用等诸多领域的新时代。本研究采用混合CR蒙特卡罗/分子动力学模拟方法，探究电荷调控（charge regulation，CR）在聚电解质（polyelectrolyte，PE）吸附到带相反电荷纳米粒子（nanoparticle，NP）的动力学过程中所起的关键作用，系统研究盐密度、聚合物链长度对PE-NP相互作用的影响；为补充CR模拟结果，还开展了恒定电荷（constant charge，CC）条件下的分子模拟。在高盐浓度下，CR会增强PE在NP表面的吸附，导致PE的回转半径快速减小；相反，CC会促使PE呈现伸展构象。在低盐或高盐浓度下，均未观察到PE链长度的明显影响；而在CC模拟中，短链PE在NP上的弛豫更快。此外，通过对比结果表明，CR条件下PE的均方位移（mean square displacement，MSD）在吸附过程中遵循更直接的路径，呈现弹道运动；而在CC条件下，无论低盐还是高盐密度，PE均表现出亚扩散行为且吸附延迟。研究结果表明，“可调控CR”是控制复杂生化环境中纳米粒子稳定性与相互作用的可靠策略。
英文摘要
Customizing the surface characteristics and stimuli-responsive behavior of nanoparticles with polyelectrolytes ushers in a new era across many aspects of our lives, ranging from advanced diagnostics to practical applications. Here, using hybrid CR Monte Carlo/ molecular dynamics simulations, we investigate how charge regulation can play a crucial role in shaping the adsorption dynamics of polyelectrolyte (PE) on oppositely charged nanoparticle (NP). We systematically investigate the influence of salt density, and polymer chain length on the PE-NP interaction. To complement CR results, we also perform molecular simulations under constant charge conditions. At high salt concentrations, CR enhances the adsorption of PE onto the NP surface, leading to a rapid decrease in the radius of gyration of PE; conversely, CC promotes the extended conformation of PE. No clear effect of PE length is observed at either low or high salt concentrations, whereas in CC simulations, the PE relaxes faster on the NP in the case of short chains. Furthermore, By comparing these results, we demonstrate that the MSD of PE follows a more direct path during adsorption implying a ballistic motion, whereas in the CC case, it exhibits subdiffusive behavior and delayed adsorption in both low and high salt density. Our findings indicates that 'tunable CR' is a robust strategy for controlling nanoparticle stability and interaction within a complex biochemical cues.
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