Correct use of excess configurational entropies to study the ideal glass transition in hard-sphere systems with continuous polydispersity

Author:

Baranau Vasili1ORCID,Tallarek Ulrich1

Affiliation:

1. Department of Chemistry, Philipps-Universität Marburg, Hans-Meerwein-Strasse 4, 35032 Marburg, Germany

Abstract

We systematically apply the resolution to the configurational entropy paradox from our previous paper [V. Baranau and U. Tallarek, J. Chem. Phys. 147, 224503 (2017)] to study configurational entropies and the glass transition in polydisperse hard-sphere systems with log-normal particle radius distributions ( r) over a wide range of polydispersities [Formula: see text]. The resolution implies the careful use of excess quantities for vibrational and configurational entropies. We obtain the fluid entropy from the fluid equation of state and the vibrational entropy from the glass equation of state; thereby, the configurational entropy becomes their difference. We discovered that the Adam–Gibbs relation is able to fit the asymptotic alpha-relaxation times τ α of the hard-sphere systems under study at high volume fractions φ when our excess configurational entropies are supplied. For polydispersity δ = 0.1, the Adam–Gibbs relation is able to fit the data over the entire range of φ studied. Ideal glass transition densities φ g obtained in this way are below predictions from the Vogel–Fulcher–Tammann fits. Our results indicate by extrapolation that the glass close packing limit φGCP for monodisperse systems is [Formula: see text], consistent with granular matter studies. Our configurational entropies extrapolated to the monodisperse case are found to match Edwards entropies from granular matter studies very well.

Publisher

AIP Publishing

Subject

General Physics and Astronomy

Cited by 1 articles. 订阅此论文施引文献 订阅此论文施引文献,注册后可以免费订阅5篇论文的施引文献,订阅后可以查看论文全部施引文献

同舟云学术

1.学者识别学者识别

2.学术分析学术分析

3.人才评估人才评估

"同舟云学术"是以全球学者为主线,采集、加工和组织学术论文而形成的新型学术文献查询和分析系统,可以对全球学者进行文献检索和人才价值评估。用户可以通过关注某些学科领域的顶尖人物而持续追踪该领域的学科进展和研究前沿。经过近期的数据扩容,当前同舟云学术共收录了国内外主流学术期刊6万余种,收集的期刊论文及会议论文总量共计约1.5亿篇,并以每天添加12000余篇中外论文的速度递增。我们也可以为用户提供个性化、定制化的学者数据。欢迎来电咨询!咨询电话:010-8811{复制后删除}0370

www.globalauthorid.com

TOP

Copyright © 2019-2024 北京同舟云网络信息技术有限公司
京公网安备11010802033243号  京ICP备18003416号-3