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Updated: Jun 25, 2025

Cooling Rate Dependent Ellipsometry Measurements to Determine the Dynamics of Thin Glassy Films
Published on: January 26, 2016
Emergent facilitation and glassy dynamics in supercooled liquids
Muhammad R Hasyim1, Kranthi K Mandadapu1,2
1Department of Chemical and Biomolecular Engineering, University of California, Berkeley, CA 94720.
This study reveals how localized bond-exchange events, or excitations, drive dynamical facilitation in supercooled liquids. Elastic interactions between these excitations explain complex glassy relaxation dynamics and super-Arrhenius temperature dependence.
Area of Science:
- Condensed Matter Physics
- Materials Science
- Statistical Mechanics
Background:
- Supercooled liquids exhibit complex dynamics, including spatially heterogeneous motion and super-Arrhenius relaxation, phenomena attributed to dynamical facilitation.
- Dynamical facilitation, where local motion triggers further motion, is crucial for understanding glassy relaxation but lacks a clear theoretical origin.
- Existing models struggle to explain the microscopic mechanisms driving facilitation and its impact on relaxation timescales.
Purpose of the Study:
- To develop a theoretical framework explaining the microscopic origins of dynamical facilitation in supercooled liquids.
- To elucidate how localized events and their interactions govern the emergent properties of glassy dynamics.
- To connect theoretical predictions with experimental and simulation observations of supercooled liquid behavior.
Main Methods:
- Developed a theory based on localized bond-exchange events (excitations) and their elastic interactions.
- Utilized the theory of linear elasticity and Markov processes to model the system.
- Simulated a model that incorporates elastic stresses and excitation interactions.
Main Results:
- The model reproduces key aspects of glassy dynamics: stretched exponential relaxation, super-Arrhenius scaling of relaxation times, and 2D finite-size effects.
- Predicted subdiffusive behavior in the mean squared displacement (MSD) at short and intermediate timescales.
- Derived phonon contributions, which, combined with excitation contributions, explain two-step relaxation and ballistic-subdiffusive-diffusive MSD crossovers.
Conclusions:
- The theory successfully explains the emergence of dynamical facilitation from localized bond-exchange events and elastic interactions.
- The model provides a unified framework for understanding diverse phenomena in supercooled liquids, from relaxation dynamics to MSD behavior.
- This work offers a microscopic basis for dynamical facilitation, advancing the understanding of glassy states.
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