A method for analyzing the non-stationary nucleation and overall transition kinetics: A case of water
Abstract
We present the statistical method as a direct extension of the mean first-passage time concept to the analysis of molecular dynamics simulation data of a phase transformation. According to the method, the mean first-passage time trajectories for the first (i = 1) as well as for the subsequent (i = 2, 3, 4,…) nucleation events should be extracted that allows one to calculate the time-dependent nucleation rate, the critical value of the order parameter (the critical size), the waiting times for the nucleation events, and the growth law of the nuclei - i.e., all the terms, which are usually necessary to characterize the overall transition kinetics. There are no restrictions in the application of the method by the specific thermodynamic regions; and the nucleation rate parameters are extracted according to their basic definitions. The method differs from the Wedekind-Bartell scheme and its modification [A. V. Mokshin and B. N. Galimzyanov, J. Phys. Chem. B 116, 11959 (2012)], where the passage-times for the first (largest) nucleus are evaluated only and where the average waiting time for the first nucleation event is accessible instead of the true steady-state nucleation time scale. We demonstrate an efficiency of the method by its application to the analysis of the vapor-to-liquid transition kinetics in water at the different temperatures. The nucleation rate/time characteristics and the droplet growth parameters are computed on the basis of the coarse-grained molecular dynamics simulation data.
- Publication:
-
Journal of Chemical Physics
- Pub Date:
- January 2014
- DOI:
- 10.1063/1.4851438
- arXiv:
- arXiv:1312.1534
- Bibcode:
- 2014JChPh.140b4104M
- Keywords:
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- Condensed Matter - Soft Condensed Matter;
- Condensed Matter - Mesoscale and Nanoscale Physics;
- Condensed Matter - Materials Science;
- Physics - Computational Physics;
- Physics - Data Analysis;
- Statistics and Probability
- E-Print:
- 15 pages, 4 figures, and 1 table