A method for analyzing the nonstationary nucleation and overall transition kinetics: A case of water
Abstract
We present the statistical method as a direct extension of the mean firstpassage time concept to the analysis of molecular dynamics simulation data of a phase transformation. According to the method, the mean firstpassage 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 timedependent 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 WedekindBartell scheme and its modification [A. V. Mokshin and B. N. Galimzyanov, J. Phys. Chem. B 116, 11959 (2012)], where the passagetimes 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 steadystate nucleation time scale. We demonstrate an efficiency of the method by its application to the analysis of the vaportoliquid 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 coarsegrained 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:

 Condensed Matter  Soft Condensed Matter;
 Condensed Matter  Mesoscale and Nanoscale Physics;
 Condensed Matter  Materials Science;
 Physics  Computational Physics;
 Physics  Data Analysis;
 Statistics and Probability
 EPrint:
 15 pages, 4 figures, and 1 table