The influence of non-stationarity and interphase curvature on the growth dynamics of spherical crystals in a metastable liquid

Philos Trans A Math Phys Eng Sci. 2021 Sep 6;379(2205):20200307. doi: 10.1098/rsta.2020.0307. Epub 2021 Jul 19.

Abstract

This manuscript is concerned with the theory of nucleation and evolution of a polydisperse ensemble of crystals in metastable liquids during the intermediate stage of a phase transformation process. A generalized growth rate of individual crystals is obtained with allowance for the effects of their non-stationary evolution in unsteady temperature (solute concentration) field and the phase transition temperature shift appearing due to the particle curvature (the Gibbs-Thomson effect) and atomic kinetics. A complete system of balance and kinetic equations determining the transient behaviour of the metastability degree and the particle-radius distribution function is analytically solved in a parametric form. The coefficient of mutual Brownian diffusion in the Fokker-Planck equation is considered in a generalized form defined by an Einstein relation. It is shown that the effects under consideration substantially change the desupercooling/desupersaturation dynamics and the transient behaviour of the particle-size distribution function. The asymptotic state of the distribution function (its 'tail'), which determines the relaxation dynamics of the concluding (Ostwald ripening) stage of a phase transformation process, is derived. This article is part of the theme issue 'Transport phenomena in complex systems (part 1)'.

Keywords: desupercooling/desupersaturation; distribution function; evolution of particulate assemblage; metastable liquid; nucleation; phase transformation.