Direct calculation of ice homogeneous nucleation rate for a molecular model of water
Abstract
Despite the importance of ice nucleation in a wide range of natural and technological systems, it is not trivial to predict its kinetics or unravel its mechanism experimentally. It is also challenging to study the stochastic nature of ice nucleation in computer simulations. The direct calculation of the nucleation rate for realistic molecular models of water is commonly regarded as one of the most challenging open problems in computational studies of water. By applying a novel coarse-graining modification to the forward-flux sampling technique, we perform the first direct rate calculation for TIP4P/Ice, one of the best existing molecular models of water. We also identify the molecular origin of the preference for the cubic polymorph during the homogeneous nucleation process.
- Publication:
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Proceedings of the National Academy of Science
- Pub Date:
- August 2015
- DOI:
- 10.1073/pnas.1509267112
- arXiv:
- arXiv:1505.01126
- Bibcode:
- 2015PNAS..11210582H
- Keywords:
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- Physics - Chemical Physics;
- Condensed Matter - Soft Condensed Matter
- E-Print:
- Main Paper: 10 pages, 6 figures, 1 table, Supplementary Information: 9 pages, 7 figures, 1 table