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Breakdown of the Stokes-Einstein relation in two, three, and four dimensions
Shiladitya Sengupta1, Smarajit Karmakar, Chandan Dasgupta
1Theoretical Sciences Unit, Jawaharlal Nehru Centre for Advanced Scientific Research, Jakkur Campus, Bangalore 560064, India.
The Journal of Chemical Physics
|April 6, 2013
Summary
The Stokes-Einstein relation breakdown in glassy liquids lessens with higher dimensions. Fragility increases with dimensionality, challenging typical associations with dynamic heterogeneity.
Area of Science:
- Condensed Matter Physics
- Materials Science
- Statistical Mechanics
Background:
- The breakdown of the Stokes-Einstein (SE) relation is a key feature of glassy dynamics in liquids.
- Theoretical models link this breakdown to dynamic heterogeneity and glass former fragility.
Purpose of the Study:
- Investigate the breakdown of the SE relation in 2, 3, and 4 dimensions.
- Understand the interrelations between SE breakdown, dynamic heterogeneity, and fragility across different spatial dimensions.
Main Methods:
- Simulations of model glass formers.
- Analysis of diffusivity and viscosity (or relaxation times).
- Calculation of dynamic heterogeneity measures.
Main Results:
- The degree of SE relation breakdown decreases as spatial dimensionality increases.
- SE breakdown in 3 and 4 dimensions explained by differences in activation free energies (Adam-Gibbs relation).
- 2D systems show deviations, explained by a generalized Adam-Gibbs relation.
Conclusions:
- SE breakdown and dynamic heterogeneity are generally correlated, with some exceptions.
- 2D systems exhibit unique behavior compared to 3D and 4D systems.
- Liquid fragility increases with dimensionality, contrary to expectations linking fragility to heterogeneity.
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