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.

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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

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article

Medium-Range Order, Density Fluctuations, and Activated Relaxation in the Equilibrated Deep Glass Regime

Kenneth S. Schweizer, Karl J. Friston
3 citations
Physical Review Letters
Material Dynamics and Properties
1.55
article

Medium-Range Order, Density Fluctuations, and Activated Relaxation in the Equilibrated Deep Glass Regime

Kenneth S. Schweizer, Karl J. Friston
article en
3 citations

Abstract

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.

Physical Review LettersVol. 134(25)
University of Illinois Urbana-Champaign (US), University of Illinois System (US)
U.S. Department of Energy, Basic Energy Sciences, Materials Research Laboratory, University of Illinois at Urbana-Champaign, Division of Materials Sciences and Engineering
Sustainable cities and communities
Openalex Percentile: Top 18%
Material Dynamics and Properties
1.55
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Medium-Range Order, Density Fluctuations, and Activated Relaxation in the Equilibrated Deep Glass Regime — Kenneth S. Schweizer, Karl J. Friston · Physical Review Letters (2025) | TGRS Research Map | TGRS