Medium-Range Order, Density Fluctuations, and Activated Relaxation in the Equilibrated Deep Glass Regime
A successful microscopic theory of activated relaxation in metastable supercooled liquids is extended to the equilibrated deep glass regime. Surprisingly, the predicted power-law scaling connections of the dynamic barrier with diverse scalar order parameters (medium-range order correlation length, dimensionless compressibility, shear modulus) remain unchanged up to astronomically long timescales, despite a fundamental crossover of equilibrium thermodynamics and structure near the laboratory kinetic vitrification point. Quantitative tests against experiments on aged to equilibrium glass-forming liquids up to nearly 20 decades in time scale reveal good agreement. This conflicts with the idea of a crossover from super-Arrhenius to literal Arrhenius relaxation around the laboratory glass transition temperature, and supports the robustness of the theoretical idea that ultraslow dynamics is causally related to medium-range structural order. New avenues of experimental and theoretical research in the deep glass regime are suggested.
Authors
- Kenneth S. Schweizer (ORCID: https://orcid.org/0000-0003-1275-3790)
- Karl J. Friston
Institutions
- University of Illinois Urbana-Champaign (US)
- University of Illinois System (US)
Publication Details
- Journal
- Physical Review Letters
- Published
- 2025-05-28
- DOI
- https://doi.org/10.1103/66zz-y23m
- Citations
- 3
- Primary Topic
- Material Dynamics and Properties
- Type
- article
- Field-Weighted Citation Impact
- 1.55
Funders
- U.S. Department of Energy
- Basic Energy Sciences
- Materials Research Laboratory, University of Illinois at Urbana-Champaign
- Division of Materials Sciences and Engineering