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arXiv 1809.02401cond-mat.stat-mech
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硬球中多体关联的形态测量方法

Morphometric approach to many-body correlations in hard spheres

Joshua F. Robinson, Francesco Turci, Roland Roth, C. Patrick Royall

摘要:

通过$n$ -体关联的\textit{morphometric}计算,我们模拟了任意体积分数下硬球液体内部局部结构的热力学。我们计算的绝对自由能的本地几何图案在良好的定量协议与分子动力学模拟在整个液体和过冷液体制度。我们发现一个双峰的密度库中的状态,其中五倍对称结构出现低于四倍对称结构的自由能,并从一个单一的反应路径预测的松弛势垒的压缩因子线性缩放。该方法提供了一个新的路线,以评估在自由能景观的变化,在体积分数动态无法访问的常规技术。

英文摘要:

We model the thermodynamics of local structures within the hard sphere liquid at arbitrary volume fractions through the \textit{morphometric} calculation of $n$-body correlations. We calculate absolute free energies of local geometric motifs in excellent quantitative agreement with molecular dynamics simulations across the liquid and supercooled liquid regimes. We find a bimodality in the density library of states where five-fold symmetric structures appear lower in free energy than four-fold symmetric structures, and from a single reaction path predict a relaxation barrier which scales linearly in the compressibility factor. The method provides a new route to assess changes in the free energy landscape at volume fractions dynamically inaccessible to conventional techniques.

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