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arXiv 0901.3169cond-mat.softcond-mat.stat-mech
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高斯核流体的异常结构和动力学

Anomalous structure and dynamics of the Gaussian-core fluid

William P. Krekelberg, Tanuj Kumar, Jeetain Mittal, Jeffrey R. Errington, Thomas M. Truskett

摘要:

已知存在高斯核(GC)流体显示异常性质的热力学状态,例如等压冷却时的膨胀(密度异常)和等温压缩时的增加的单粒子流动性(自扩散率异常)。我们研究了温度和密度如何影响其短程平移结构序,其特征在于两体过剩熵。我们发现,有一个广泛的条件下,短程平移秩序的GC流体等温压缩后减少(结构秩序异常)。构造异常的起源在性质上与其他异常流体相似,并与压缩如何影响不同长度尺度的静态相关性有关。我们发现,GC流体的自扩散率服从标度关系的两体过剩熵是非常相似的观察到的各种简单的液体。这种关系的一个结果是,状态点的结构,自扩散,和密度异常的高斯核心流体出现级联区域的温度-密度平面上,一种现象观察到较早的水状流体模型。有,但是,GC和类水流体的异常之间的关键差异,我们讨论如何可以定性地理解这些模型考虑各自的粒子间电位。最后,我们注意到,高斯核流体的自扩散率服从不同的标度律取决于是否考虑两体或总过剩熵。这一发现,这值得更全面的未来研究,似乎强调了更高的身体相关性的流体与有界相互作用的行为的意义。

英文摘要:

It is known that there are thermodynamic states for which the Gaussian-core (GC) fluid displays anomalous properties such as expansion upon isobaric cooling (density anomaly) and increased single-particle mobility upon isothermal compression (self-diffusivity anomaly). We investigate how temperature and density affect its short-range translational structural order, as characterized by the two-body excess entropy. We find that there is a wide range of conditions for which the short-range translational order of the GC fluid decreases upon isothermal compression (structural order anomaly). The origin of the structural anomaly is qualitatively similar to that of other anomalous fluids and is connected to how compression affects static correlations at different length scales. We find that the self-diffusivity of the GC fluid obeys a scaling relationship with the two-body excess entropy that is very similar to the one observed for a variety of simple liquids. One consequence of this relationship is that the state points for which structural, self-diffusivity, and density anomalies of the Gaussian-core fluid occur appear as cascading regions on the temperature-density plane, a phenomenon observed earlier for models of waterlike fluids. There are, however, key differences between the anomalies of GC and waterlike fluids, and we discuss how those can be qualitatively understood by considering the respective interparticle potentials of these models. Finally, we note that the self-diffusivity of the Gaussian-core fluid obeys different scaling laws depending on whether the two-body or total excess entropy is considered. This finding, which deserves more comprehensive future study, appears to underscore the significance of higher-body correlations for the behavior of fluids with bounded interactions.

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