论文标题

二元Voronoi流体的玻璃动力学:模式耦合分析

Glassy dynamics of a binary Voronoi fluid: A mode-coupling analysis

论文作者

Ruscher, Céline, Ciarella, Simone, Luo, Chengjie, Janssen, Liesbeth M. C., Farago, Jean, Baschnagel, Jörg

论文摘要

二元Voronoi混合物是一种流体模型,其相互作用是局部和多体。在这里,我们对弱分散和添加剂的等摩尔混合物进行分子动力学(MD)模拟。我们第一次研究该混合物在超冷液体方面的结构松弛。从模拟中,我们确定了大量波向量的时间和温度依赖性散射函数,以及两个粒子物种的平均值位移。我们通过将MD结果与基于第一原理的理想模式耦合理论(MCT)进行比较,对动力学进行了详细的分析。为此,我们采用了两种方法:拟合理论的渐近预测,以及基于模拟中静态结构因素输入的无拟合参数MCT计算。我们发现,相对于与配对相互作用的简单液体进行的相似分析,Voronoi混合物的多体相互作用不会导致质量差异很强。 For instance, the fits give an exponent parameter $λ\approx 0.746$ comparable to typical values found for simple liquids, the wavevector dependence of the Kohlrausch relaxation time is in good agreement with literature results for polydisperse hard spheres, and the MCT calculations based on static input overestimate the critical temperature, albeit only by a factor of about 1.2.相对于其他研究过的超冷液模型,例如二进制KOB - Andersen Lennard-Jones混合物,这种高估似乎是弱的。总体而言,MCT和仿真之间的一致性表明,即使系统本身受许多体型相互作用,即使系统本身依赖于静态的两点结构相关性,也可以仅基于静态的两点结构相关性来预测具有定性的几种微观动态特性,并且在某些情况下仅基于静态的两点结构相关性。

The binary Voronoi mixture is a fluid model whose interactions are local and many-body. Here we perform molecular-dynamics (MD) simulations of an equimolar mixture that is weakly polydisperse and additive. For the first time we study the structural relaxation of this mixture in the supercooled-liquid regime. From the simulations we determine the time- and temperature-dependent scattering functions for a large range of wave vectors, as well as the mean-square displacements of both particle species. We perform a detailed analysis of the dynamics by comparing the MD results with the first-principles-based idealized mode-coupling theory (MCT). To this end, we employ two approaches: fits to the asymptotic predictions of the theory, and fit-parameter-free binary MCT calculations based on static-structure-factor input from the simulations. We find that many-body interactions of the Voronoi mixture do not lead to strong qualitative differences relative to similar analyses carried out for simple liquids with pair-wise interactions. For instance, the fits give an exponent parameter $λ\approx 0.746$ comparable to typical values found for simple liquids, the wavevector dependence of the Kohlrausch relaxation time is in good agreement with literature results for polydisperse hard spheres, and the MCT calculations based on static input overestimate the critical temperature, albeit only by a factor of about 1.2. This overestimation appears to be weak relative to other well-studied supercooled-liquid models such as the binary Kob--Andersen Lennard-Jones mixture. Overall, the agreement between MCT and simulation suggests that it is possible to predict several microscopic dynamic properties with qualitative, and in some cases near-quantitative, accuracy based solely on static two-point structural correlations, even though the system itself is inherently governed by many-body interactions.

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