Transformations of the distribution of nuclei formed in a nucleation pulse: Interface-limited growth

A typical nucleation-growth process is considered: a system is quenched into a supersaturated state with a small critical radius r( *) (-) and is allowed to nucleate during a finite time interval t(n), after which the supersaturation is abruptly reduced to a fixed value with a larger critical radius r( *) (+). The size-distribution of nucleated particles f(r,t) further evolves due to their deterministic growth and decay for r larger or smaller than r( *) (+), respectively. A general analytic expressions for f(r,t) is obtained, and it is shown that after a large growth time t this distribution approaches an asymptotic shape determined by two dimensionless parameters, lambda related to t(n), and Lambda=r( *) (+)/r( *) (-). This shape is strongly asymmetric with an exponential and double-exponential cutoffs at small and large sizes, respectively, and with a broad near-flat top in case of a long pulse. Conversely, for a short pulse the distribution acquires a distinct maximum at r=r(max)(t) and approaches a universal shape exp[zeta-e(zeta)], with zeta proportional to r-r(max), independent of the pulse duration. General asymptotic predictions are examined in terms of Zeldovich-Frenkel nucleation model where the entire transient behavior can be described in terms of the Lambert W function. Modifications for the Turnbull-Fisher model are also considered, and analytics is compared with exact numerics. Results are expected to have direct implementations in analysis of two-step annealing crystallization experiments, although other applications might be anticipated due to universality of the nucleation pulse technique.