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Composition and concentration anomalies for structure and dynamics of Gaussian-core mixtures

机译:结构和动力学的组成和浓度异常   高斯核心混合物

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摘要

We report molecular dynamics simulation results for two-component fluidmixtures of Gaussian-core particles, focusing on how tracer diffusivities andstatic pair correlations depend on temperature, particle concentration, andcomposition. At low particle concentrations, these systems behave like simpleatomic mixtures. However, for intermediate concentrations, the single-particledynamics of the two species largely decouple, giving rise to the followinganomalous trends. Increasing either the concentration of the fluid (at fixedcomposition) or the mole fraction of the larger particles (at fixed particleconcentration) enhances the tracer diffusivity of the larger particles, butdecreases that of the smaller particles. In fact, at sufficiently high particleconcentrations, the larger particles exhibit higher mobility than the smallerparticles. Each of these dynamic behaviors is accompanied by a correspondingstructural trend that characterizes how either concentration or compositionaffects the strength of the static pair correlations. Specifically, the dynamictrends observed here are consistent with a single empirical scaling law thatrelates an appropriately normalized tracer diffusivity to its pair-correlationcontribution to the excess entropy.
机译:我们报告了高斯核颗粒的两组分流体混合物的分子动力学模拟结果,重点是示踪剂扩散率和静态对相关性如何取决于温度,颗粒浓度和组成。在低颗粒浓度下,这些系统的行为类似于简单原子混合物。然而,对于中等浓度,两个物种的单粒子动力学很大程度上解耦,从而引起以下异常趋势。增加流体的浓度(以固定的组成)或增大较大颗粒的摩尔分数(以固定的颗粒浓度)会增加较大颗粒的示踪剂扩散率,但会减小较小颗粒的示踪剂扩散率。实际上,在足够高的颗粒浓度下,较大的颗粒表现出比较小的颗粒更高的迁移率。这些动态行为中的每一个都伴随着一个相应的结构趋势,该趋势描述了浓度或组成如何影响静态对相关的强度。具体而言,此处观察到的动态趋势与单个经验定标定律相一致,该定律定律将适当归一化的示踪剂扩散率与其对过量熵的对相关贡献相关联。

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