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Published on: October 31, 2019
Crystal nucleation in a supercooled liquid with glassy dynamics.
Ivan Saika-Voivod1, Richard K Bowles, Peter H Poole
1Department of Physics and Physical Oceanography, Memorial University of Newfoundland, St. John's, NL, A1B 3X7, Canada.
Physical Review Letters
|April 7, 2010
Summary
Supercooled liquid silica crystallizes rapidly below its homogeneous nucleation limit (HNL). Glassy dynamics, not just temperature, dictates this limit, influencing silica
Area of Science:
- Condensed matter physics
- Materials science
- Computational chemistry
Background:
- Supercooled liquids exhibit complex dynamics and can form glasses.
- Silica is a model glass-forming material with technological applications.
- Understanding crystallization limits is crucial for glass and materials science.
Purpose of the Study:
- Investigate the interplay between glassy dynamics and crystallization in supercooled liquid silica.
- Determine the homogeneous nucleation limit (HNL) for silica.
- Explore the role of the Stokes-Einstein relation in setting crystallization boundaries.
Main Methods:
- Molecular dynamics simulations of supercooled, high-density liquid silica.
- Analysis of temperature-dependent dynamics, including crystal nucleation rates.
- Examination of the Stokes-Einstein relation and its breakdown.
- Comparison with theoretical concepts like the Kauzmann temperature and spinodal effects.
Main Results:
- Identified a temperature range exhibiting both crystal nucleation and glass-like dynamics.
- Established a homogeneous nucleation limit (HNL) below which liquid silica crystallizes too rapidly to equilibrate.
- Demonstrated that the HNL is influenced by the breakdown of the Stokes-Einstein relation, highlighting the importance of glassy dynamics.
- Observed spinodal-like effects near the HNL.
Conclusions:
- Glassy dynamics play a critical role in defining the crystallization limit of supercooled liquid silica.
- The homogeneous nucleation limit is not solely determined by temperature but also by liquid dynamics.
- Further research into the relationship between dynamic heterogeneity and phase transitions in glass-forming liquids is warranted.
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