示踪添加剂周围溶剂化壳层的调谐结构和迁移率
Tuning structure and mobility of solvation shells surrounding tracer additives
摘要：
分子动力学模拟和随机Fokker-Planck方程为基础的方法被用来阐明当示踪剂-溶剂相互作用被合理地修改以影响相应的溶剂化结构时，一个或多个示踪剂粒子附近的位置依赖性溶剂迁移率是如何受到影响的。对于致密硬球流体中的示踪剂，我们比较了两种类型的示踪剂-溶剂相互作用：（1）硬球样相互作用;以及（2）经由统计力学理论设计的延伸超出硬核的软排斥，以通过抑制配位壳结构来增强无限稀释下的示踪剂迁移率（Carmer等人，软物质8（2011））。对于后者的情况下，我们表明，周围的溶剂颗粒的流动性也增加了通过添加的软排斥相互作用，这有助于合理化的示踪剂的增强扩散的机制。然而，如果多个示踪剂表面更接近（如在更高的示踪剂浓度），类似的相互作用，破坏局部溶剂化结构，而不是抑制位置依赖的溶剂动力学。
英文摘要：
Molecular dynamics simulations and a stochastic Fokker-Planck equation based approach are used to illuminate how position-dependent solvent mobility near one or more tracer particle(s) is affected when tracer-solvent interactions are rationally modified to affect corresponding solvation structure. For tracers in a dense hard-sphere fluid, we compare two types of tracer-solvent interactions: (1) a hard-sphere-like interaction; and (2) a soft repulsion extending beyond the hard core designed via statistical mechanical theory to enhance tracer mobility at infinite dilution by suppressing coordination-shell structure (Carmer et al., Soft Matter 8 (2011)). For the latter case, we show that the mobility of surrounding solvent particles is also increased by addition of the soft repulsive interaction, which helps to rationalize the mechanism underlying the tracer's enhanced diffusivity. However, if multiple tracer surfaces are in closer proximity (as at higher tracer concentrations), similar interactions that disrupt local solvation structure instead suppress the position-dependent solvent dynamics.
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