Time-dependent distributions in self-quenching nucleation

Diffusion- and interface-limited Becker-Döring (BD) -type nucleation is considered in a closed system, where supersaturation is depleted by growing nuclei. Special focus is on nonadiabatic effects, which become increasingly pronounced for barriers lower than 20-25k_BT, and which lead to nucleation rates deviating from their quasi-steady-state (QSS) values. Several essential modifications of the QSS distribution are observed. For example, the front is continuous rather than sharp and has a double-exponential shape, which is in agreement with the earlier matched asymptotic solution obtained in neglect of depletion. The total number of nuclei is larger than predicted by the QSS approximation. The obtained distributions are compared with numerical solutions of the BD equations and can serve as initial conditions for further transition to the Ostwald Ripening stage.