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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7 March 2024
Research Article|
March 06 2024
Viscoelastic relaxation and topological fluctuations in glass-forming liquids
Chi-Huan Tung
;
Chi-Huan Tung
(Data curation, Formal analysis, Investigation, Methodology, Writing – original draft)
1
Department of Materials Science and Engineering, National Tsing Hua University
, Hsinchu 300044, Taiwan
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Shou-Yi Chang
;
Shou-Yi Chang
(Supervision, Writing – review & editing)
1
Department of Materials Science and Engineering, National Tsing Hua University
, Hsinchu 300044, Taiwan
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Sidney Yip;
Sidney Yip
(Formal analysis, Investigation, Writing – review & editing)
2
Department of Nuclear Science and Engineering, Massachusetts Institute of Technology
, Cambridge, Massachusetts 02139, USA
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Yangyang Wang
;
Yangyang Wang
a)
(Investigation, Writing – review & editing)
3
Center for Nanophase Materials Sciences, Oak Ridge National Laboratory
, Oak Ridge, Tennessee 37831, USA
a)Author to whom correspondence should be addressed: [email protected]
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Jan-Michael Y. Carrillo
;
Jan-Michael Y. Carrillo
(Data curation, Investigation, Writing – review & editing)
3
Center for Nanophase Materials Sciences, Oak Ridge National Laboratory
, Oak Ridge, Tennessee 37831, USA
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Bobby G. Sumpter
;
Bobby G. Sumpter
(Supervision, Writing – review & editing)
3
Center for Nanophase Materials Sciences, Oak Ridge National Laboratory
, Oak Ridge, Tennessee 37831, USA
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Yuya Shinohara
;
Yuya Shinohara
(Investigation, Writing – review & editing)
4
Materials Science and Technology Division, Oak Ridge National Laboratory
, Oak Ridge, Tennessee 37831, USA
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Changwoo Do
;
Changwoo Do
(Investigation, Writing – review & editing)
5
Neutron Scattering Division, Oak Ridge National Laboratory
, Oak Ridge, Tennessee 37831, USA
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Wei-Ren Chen
Wei-Ren Chen
b)
(Conceptualization, Data curation, Formal analysis, Investigation, Methodology, Supervision, Writing – review & editing)
5
Neutron Scattering Division, Oak Ridge National Laboratory
, Oak Ridge, Tennessee 37831, USA
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a)Author to whom correspondence should be addressed: [email protected]
b)
Electronic mail: [email protected]
J. Chem. Phys. 160, 094506 (2024)
Article history
Received:
December 01 2023
Accepted:
February 17 2024
Citation
Chi-Huan Tung, Shou-Yi Chang, Sidney Yip, Yangyang Wang, Jan-Michael Y. Carrillo, Bobby G. Sumpter, Yuya Shinohara, Changwoo Do, Wei-Ren Chen; Viscoelastic relaxation and topological fluctuations in glass-forming liquids. J. Chem. Phys. 7 March 2024; 160 (9): 094506. https://doi.org/10.1063/5.0189938
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