From nucleation and coarsening to coalescence in metastable liquids

Abstract

The transition of a metastable liquid (supersaturated solution or supercooled melt) occurring from the intermediate stage (where the crystals nucleate and grow) to the concluding stage (where the larger particles evolve at the expense of the dissolution of smaller particles) is theoretically described, with allowance for various mass transfer mechanisms (reaction on the interface surface, volume diffusion, grain-boundary diffusion, diffusion along the dislocations) arising at the stage of Ostwald ripening (coalescence). The initial distribution function (its 'tail') for the concluding stage (forming as a result of the evolution of a particulate assemblage during the intermediate stage) is taken into account to determine the particle-size distribution function at the stage of Ostwald ripening. This modified distribution function essentially differs from the universal Lifshitz-Slyozov (LS) solutions for several mass transfer mechanisms. Namely, its maximum lies below and is shifted to the left in comparison with the LS asymptotic distribution function. In addition, the right branch of the particle-size distribution lies above and is shifted to the right of the LS blocking point. It is shown that the initial 'tail' of the particle-size distribution function completely determines its behaviour at the concluding stage of Ostwald ripening. The present theory agrees well with experimental data. © 2020 The Author(s) Published by the Royal Society. All rights reserved.