Viscoelastic relaxation and topological fluctuations in glass-forming liquids

Tung, Chi-Huan; Chang, Shou-Yi; Yip, Sidney; Wang, Yangyang; Carrillo, Jan-Michael Y.; Sumpter, Bobby G.; Shinohara, Yuya; Do, Changwoo; Chen, Wei-Ren

doi:10.1063/5.0189938

Title: Viscoelastic relaxation and topological fluctuations in glass-forming liquids

Journal Article · 05 March 2024 · Journal of Chemical Physics

DOI: https://doi.org/10.1063/5.0189938 · OSTI ID:2324056

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^[1]; Yip, Sidney ^[2];

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National Tsing Hua Univ., Hsinchu (Taiwan)
Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States)
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Sciences (CNMS)
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)

In this study, a method for characterizing the topological fluctuations in liquids is proposed. This approach exploits the concept of the weighted gyration tensor of a collection of particles and permits the definition of a local configurational unit (LCU). The first principal axis of the gyration tensor serves as the director of the LCU, which can be tracked and analyzed by molecular dynamics simulations. Analysis of moderately supercooled Kob–Andersen mixtures suggests that orientational relaxation of the LCU closely follows viscoelastic relaxation and exhibits a two-stage behavior. The slow relaxing component of the LCU corresponds to the structural, Maxwellian mechanical relaxation. Additionally, it is found that the mean curvature of the LCUs is approximately zero at the Maxwell relaxation time with the Gaussian curvature being negative. This observation implies that structural relaxation occurs when the configurationally stable and destabilized regions interpenetrate each other in a bicontinuous manner. Finally, the mean and Gaussian curvatures of the LCUs can serve as reduced variables for the shear stress correlation, providing a compelling proof of the close connection between viscoelastic relaxation and topological fluctuations in glass-forming liquids.

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Research Organization:: Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Spallation Neutron Source (SNS); Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Sciences (CNMS)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division (MSE); Ministry of Science and Technology of Taiwan (MOST)

Grant/Contract Number:: AC05-00OR22725

OSTI ID:: 2324056

Alternate ID(s):: OSTI ID: 2538506

Journal Information:: Journal of Chemical Physics, Journal Name: Journal of Chemical Physics Journal Issue: 9 Vol. 160; ISSN 0021-9606

Publisher:: American Institute of Physics (AIP)Copyright Statement

Country of Publication:: United States

Language:: English

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
Molecular dynamics
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Title: Viscoelastic relaxation and topological fluctuations in glass-forming liquids

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References (63)

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