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 ($i=2$, $3$, $4$, $\dots$) 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, B.N. Galimzyanov, J. Phys. Chem. B {\bf 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.

15 pages, 4 figures, and 1 table

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• Caveats of mean first-passage time methods applied to the crystallization transition: effects of non-Markovianity
• Cavity nucleation in single-component homogeneous amorphous solids under negative pressure
• Is there a one-to-one correspondence between interparticle interactions and physical properties of liquid?