Method to estimate crystal/liquid surface energy by dissolution of subcritical nuclei

Within the framework of the classical nucleation theory (CNT) the nucleus–liquid surface energy (σ) is one of the most important parameters to predict or analyze nucleation kinetics in undercooled liquids. However, the few methods proposed to determine σ are based on the direct use of nucleation rate data and, thus, do not allow an independent test of the theory. In the present paper, this parameter is estimated without direct use of nucleation rate data. Instead, we provide further experimental evidence for the dissolution of sub-critical nuclei at several development temperatures and use this effect to estimate the nucleus–liquid surface energy. The results of the present analysis demonstrate that, in agreement with a new approach for the description of nucleation processes, not only the surface energy but also the driving force for nucleation have quite different values from those of the evolving macrophases. The possible implications of this result for the understanding of crystal nucleation in liquids are discussed.