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Local-Average Free Volume Correlates with Dynamics in Glass Formers

Mei, Baicheng and Zhuang, Bilin and Lu, Yuyuan and An, Lijia and Wang, Zhen-Gang (2022) Local-Average Free Volume Correlates with Dynamics in Glass Formers. Journal of Physical Chemistry Letters, 13 (17). pp. 3957-3964. ISSN 1948-7185. doi:10.1021/acs.jpclett.2c00072.

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Glass formers exhibit a pronounced slowdown in dynamics, accompanied by progressive heterogeneity as they approach the glass transition. There is intense debate over whether the dramatic slowdown is caused by dynamical heterogeneity and whether the enhanced dynamical heterogeneity originates from structural causes. However, the connection between dynamical heterogeneity and the spatial distribution of the single-particle free volume (a purely static structural quantity) was found to be rather weak, which raises the question of whether dynamic heterogeneity has a purely structural origin. Here, by introducing the concept of local-average free volume, we present numerical evidence that long-time dynamic heterogeneity shows significantly enhanced correlation with the average local free volume over a length scale of a few neighboring shells. Our results resolve the long-standing controversy about whether free volume plays an important role in particle rearrangements associated with the activated hopping relaxation. The concept of “local average” can be applied to other local structural descriptors to better correlate with dynamic heterogeneity in glass-forming liquids.

Item Type:Article
Related URLs:
URLURL TypeDescription
Mei, Baicheng0000-0003-0289-248X
Zhuang, Bilin0000-0003-2934-4264
Lu, Yuyuan0000-0002-4073-678X
Wang, Zhen-Gang0000-0002-3361-6114
Additional Information:© 2022 American Chemical Society. Received 10 January 2022. Accepted 5 April 2022. Published online 28 April 2022. Published in issue 5 May 2022. This work was supported by the National Key R&D Program of China (Grant 2020YFA0713601) and the National Natural Science Foundation of China (Grants 21790340 and 22073092). Additional support for Y.L. was provided by the Youth Innovation Promotion Association of CAS (Grant Y202054). Z.-G.W. acknowledges financial support from the Hong Kong Quantum AI Lab Ltd. The authors declare no competing financial interest.
Funding AgencyGrant Number
Ministry of Science and Technology (China)2020YFA0713601
National Natural Science Foundation of China21790340
National Natural Science Foundation of China22073092
Chinese Academy of SciencesY202054
Hong Kong Quantum AI Lab LtdUNSPECIFIED
Subject Keywords:Amorphous materials, Cluster chemistry, Liquids, Physical and chemical properties, Rearrangement
Issue or Number:17
Record Number:CaltechAUTHORS:20220520-388267000
Persistent URL:
Official Citation:Local-Average Free Volume Correlates with Dynamics in Glass Formers Baicheng Mei, Bilin Zhuang, Yuyuan Lu, Lijia An, and Zhen-Gang Wang The Journal of Physical Chemistry Letters 2022 13 (17), 3957-3964 DOI: 10.1021/acs.jpclett.2c00072
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:114844
Deposited By: George Porter
Deposited On:20 May 2022 22:22
Last Modified:20 May 2022 22:22

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