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Effect of total and pair configurational entropy in determining dynamics of supercooled liquids over a range of densities

机译:总和对配置熵在确定动力学中的作用   在一系列密度范围内的过冷液体

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摘要

In this paper, we present a study of supercooled liquids interacting with theLennard Jones (LJ) potential and the corresponding purely repulsive(Weeks-Chandler-Andersen or WCA) potential, over a range of densities andtemperatures, in order to understand the origin of their different dynamics inspite of their structures being similar. Using the configurational entropy asthe thermodynamic marker via the Adam Gibbs (AG) relation, we show that thedifference in the dynamics of these two systems at low temperatures can beexplained from thermodynamics. At higher densities both the thermodynamical anddynamical difference between these model systems decrease, which isquantitatively demonstrated in this paper by calculating different parameters.The study also reveals the origin of the difference in pair entropy despite thesimilarity in the structure. Although the maximum difference in structure isobtained in the partial radial distribution function (rdf) of the B type ofparticles, the rdf of AA pairs and AB pairs give rise to the differences in theentropy and dynamics. This work supports the observation made in an earlierstudy (Phys. Rev. Lett.,\textbf {113}, 225701, 2014) and shows that they aregeneric in nature, independent of density.
机译:在本文中,我们对过冷液体在一定的密度和温度范围内与伦纳德·琼斯(LJ)电位和相应的纯斥力(Weeks-Chandler-Andersen或WCA)相互作用进行了研究,以了解它们的起源。尽管它们的结构相似,但它们具有不同的动力学。通过亚当·吉布斯(AG)关系使用构型熵作为热力学标记,我们证明了这两个系统在低温下的动力学差异可以从热力学中得到解释。在较高的密度下,这些模型系统之间的热力学和动力学差异都会减小,本文通过计算不同的参数定量地证明了这一点。研究还揭示了尽管结构相似,但对熵差异的起源。尽管在B型颗粒的部分径向分布函数(rdf)中获得了最大的结构差异,但AA对和AB对的rdf引起了熵和动力​​学的差异。这项工作支持了早期研究中的观察(Phys。Rev. Lett。,\ textbf {113},225701,2014),并表明它们本质上是通用的,与密度无关。

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