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Static self-induced heterogeneity in glass-forming liquids: Overlap as a microscope
Benjamin Guiselin1, Gilles Tarjus2, Ludovic Berthier1
1Laboratoire Charles Coulomb (L2C), Université de Montpellier, CNRS, 34095 Montpellier, France.
The Journal of Chemical Physics
|May 21, 2022
Summary
This study introduces a new method to visualize and quantify heterogeneity in glass-forming liquids. It measures overlap fluctuations in cavities, providing insights into configurational entropy and amorphous state surface tension.
Area of Science:
- Condensed Matter Physics
- Statistical Mechanics
- Materials Science
Background:
- Glass-forming liquids exhibit complex heterogeneity.
- Understanding this heterogeneity is crucial for theories of glass formation.
Purpose of the Study:
- To develop and implement a local probe for static self-induced heterogeneity in glass-forming liquids.
- To directly detect spatial variations in overlap fluctuations and analyze configurational entropy.
Main Methods:
- Numerical implementation of a local probe using equilibrium statistics.
- Measurement of overlap between configurations in mesoscopic cavities.
- Systematic variation of cavity location to map heterogeneity.
Main Results:
- Direct detection of spatial variations in overlap fluctuations.
- Detailed analysis of local configurational entropy statistics.
- Inference of surface tension between amorphous states.
Conclusions:
- The study provides the first direct visualization and quantification of self-induced heterogeneity in glass formation.
- Results support the random first-order transition theory of glass formation.
- Paves the way for coarse-grained theories and assessing thermodynamics in supercooled liquids.

