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Configurational entropy of polydisperse supercooled liquids
The Journal of Chemical Physics ( IF 3.1 ) Pub Date : 2018-10-15 , DOI: 10.1063/1.5040975
Misaki Ozawa 1 , Giorgio Parisi 2 , Ludovic Berthier 1
Affiliation  

We propose a computational method to measure the configurational entropy in generic polydisperse glass-formers. In particular, our method resolves issues related to the diverging mixing entropy term due to a continuous polydispersity. The configurational entropy is measured as the difference between the well-defined fluid entropy and a more problematic glass entropy. We show that the glass entropy can be computed by a simple generalisation of the Frenkel-Ladd thermodynamic integration method, which takes into account permutations of the particle diameters. This approach automatically provides a physically meaningful mixing entropy for the glass entropy and includes contributions that are not purely vibrational. The proposed configurational entropy is thus devoid of conceptual and technical difficulties due to continuous polydispersity, while being conceptually closer, but technically simpler, than alternative free energy approaches.

中文翻译:

多分散过冷液体的结构熵

我们提出了一种计算方法来测量通用的多分散玻璃形成剂中的结构熵。尤其是,我们的方法解决了由于连续的多分散性而导致的混合熵项发散的问题。构型熵被测量为定义明确的流体熵和更多问题玻璃熵之间的差。我们表明,可以通过将颗粒直径的排列考虑在内的Frenkel-Ladd热力学积分方法的简单概括来计算玻璃的熵。这种方法自动为玻璃熵提供了一个物理上有意义的混合熵,并且包括了并非纯振动的贡献。因此,由于连续的多分散性,所提出的构型熵没有概念和技术上的困难,
更新日期:2018-10-19
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