Igniting homogeneous nucleation

Abstract

Transient homogeneous nucleation is studied in the limit of large critical sizes. Starting from pure monomers, three eras of transient nucleation are characterized in the classic Becker-Döring kinetic equations with two different models of discrete diffusivity: the classic Turnbull-Fisher formula and an expression describing thermally driven growth of the nucleus. The latter diffusivity yields time lags for nucleation which are much closer to values measured in experiments with disilicate glasses. After an initial stage in which the number of monomers decreases, many clusters of small size are produced and a continuous size distribution is created. During the second era, nucleii are increasing steadily in size in such a way that their distribution appears as a wave front advancing towards the critical size for steady nucleation. The nucleation rate at critical size is negligible during this era. After the wave front reaches critical size, it ignites the creation of supercritical clusters at a rate that increases monotonically until its steady value is reached. Analytical formulas for the transient nucleation rate and the time lag are obtained that improve classical ones and compare very well with direct numerical solutions.