Understanding Relaxation in the Kob-Andersen Liquid Based on Entropy, String, Shoving, Localization, and Parabolic Models

• Published in: The journal of physical chemistry. B 2024-11, Vol.128 (44), p.10999-11021
• Main Authors: Yuan, Qi-Lu, Xu, Xiaolei, Douglas, Jack F., Xu, Wen-Sheng
• Format: Article
• Language: English
• Subjects: B: Soft Matter, Fluid Interfaces, Colloids, Polymers, and Glassy Materials
• ISSN: 1520-6106; 1520-5207; 1520-5207
• DOI: 10.1021/acs.jpcb.4c04806

We assess the validity of a range of models of glass formation based on molecular dynamics simulation results of the Kob-Andersen (KA) model system under a wide range of constant volume and constant pressure conditions. These models include the Adam–Gibbs model emphasizing configurational entropy, the string model emphasizing collective particle exchange motion, the shoving model emphasizing material elasticity, the localization model emphasizing dynamical free volume, and parabolic models based on the ideas of dynamic facilitation and, alternatively, the hypothesis that glass formation involves an avoided critical point. We demonstrate that these seemingly disparate models all provide a reasonable description of structural relaxation and diffusion data for the KA model system under all simulation conditions considered. Hence, the present study points to some unity in our understanding of the relationship between leading models of glass formation, supporting inferences drawn from previous studies of polymeric glass-forming liquids.