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Self-Induced Heterogeneity in Deeply Supercooled Liquids
1Laboratoire Charles Coulomb (L2C), Université de Montpellier, CNRS, 34095 Montpellier, France and Yusuf Hamied Deprtment of Chemistry, University of Cambridge, Lensfield Road, Cambridge CB2 1EW, United Kingdom.
Physical Review Letters
|September 3, 2021
Summary
Computer simulations reveal that spatial inhomogeneities in supercooled liquids, crucial for understanding the glass transition, exhibit broad thermodynamic and dynamic fluctuations. These fluctuations correlate, supporting a thermodynamic origin for slow liquid dynamics.
Area of Science:
- Condensed Matter Physics
- Computational Materials Science
- Statistical Mechanics
Background:
- Deeply supercooled liquids exhibit complex properties arising from self-induced, transient, and nanoscopic spatial inhomogeneities.
- Theoretical treatment of these systems is challenging due to the dynamic and heterogeneous nature of their structure.
- Understanding the approach to the experimental glass transition requires analyzing these inherent inhomogeneities.
Purpose of the Study:
- To analyze self-induced static and dynamic heterogeneity in equilibrium systems near the glass transition using computer simulations.
- To characterize sample-to-sample fluctuations in dynamic and thermodynamic properties within mesoscopic systems.
- To investigate the correlation between dynamic and thermodynamic fluctuations and their implications for slow dynamics.
Main Methods:
- Utilized extensive computer simulations of equilibrium systems approaching the glass transition.
- Analyzed spatial inhomogeneities, including static and dynamic heterogeneity.
- Characterized local lifetimes and distributions of dynamic heterogeneity.
- Quantified thermodynamic fluctuations and their relationship with dynamic properties.
Main Results:
- Observed broad sample-to-sample fluctuations in both dynamic and thermodynamic properties of mesoscopic systems.
- Findings on local lifetimes and dynamic heterogeneity distributions align well with recent single-molecule experimental studies.
- Discovered surprisingly broad thermodynamic fluctuations that correlate strongly with dynamic fluctuations.
Conclusions:
- The study provides a local, simulation-based test supporting a thermodynamic origin for the slow dynamics observed in supercooled liquids.
- The observed correlations between dynamic and thermodynamic heterogeneity offer new insights into the fundamental nature of the glass transition.
- Computer simulations are a powerful tool for unraveling the complex behavior of supercooled liquids.
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