We propose and numerically implement a local probe of the static self-induced heterogeneity characterizing glass-forming liquids. This method relies on the equilibrium statistics of the overlap between pairs of configurations measured in mesoscopic cavities with unconstrained boundaries. By systematically changing the location of the probed cavity, we directly detect spatial variations of the overlap fluctuations. We provide a detailed analysis of the statistics of a local estimate of the configurational entropy, and we infer an estimate of the surface tension between amorphous states, ingredients that are both at the basis of the random first-order transition theory of glass formation. Our results represent the first direct attempt to visualize and quantify the self-induced heterogeneity underpinning the thermodynamics of glass formation. They pave the way for the development of coarse-grained effective theories and for a direct assessment of the role of thermodynamics in the activated dynamics of deeply supercooled liquids.
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21 May 2022
Research Article|
May 17 2022
Static self-induced heterogeneity in glass-forming liquids: Overlap as a microscope
Special Collection:
Slow Dynamics
Benjamin Guiselin
;
Benjamin Guiselin
1
Laboratoire Charles Coulomb (L2C), Université de Montpellier, CNRS
, 34095 Montpellier, France
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Gilles Tarjus;
Gilles Tarjus
2
LPTMC, CNRS-UMR 7600, Sorbonne Université
, 4 Pl. Jussieu, F-75005 Paris, France
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Ludovic Berthier
Ludovic Berthier
a)
1
Laboratoire Charles Coulomb (L2C), Université de Montpellier, CNRS
, 34095 Montpellier, France
3
Yusuf Hamied Department of Chemistry, University of Cambridge
, Lensfield Road, Cambridge CB2 1EW, United Kingdom
a)Author to whom correspondence should be addressed: ludovic.berthier@umontpellier.fr
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a)Author to whom correspondence should be addressed: ludovic.berthier@umontpellier.fr
Note: This paper is part of the JCP Special Topic on Slow Dynamics.
J. Chem. Phys. 156, 194503 (2022)
Article history
Received:
January 26 2022
Accepted:
April 18 2022
Citation
Benjamin Guiselin, Gilles Tarjus, Ludovic Berthier; Static self-induced heterogeneity in glass-forming liquids: Overlap as a microscope. J. Chem. Phys. 21 May 2022; 156 (19): 194503. https://doi.org/10.1063/5.0086517
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