Homogeneous nucleation of NaCl in supersaturated solutions

The seeding method is an approximate approach to investigate nucleation that combines molecular dynamics simulations with classical nucleation theory. Recently, this technique has been successfully implemented in a broad range of nucleation studies. However, its accuracy is subject to the arbitrary choice of the order parameter threshold used to distinguish liquid-like from solid-like molecules. We revisit here the crystallization of NaCl from a supersaturated brine solution and show that consistency between seeding and rigorous methods, like Forward Flux Sampling (from previous work) or spontaneous crystallization (from this work), is achieved by following a mislabelling criterion to select such threshold (i.e. equaling the fraction of the mislabelled particles in the bulk parent and nucleating phases). This work supports the use of seeding to obtain fast and reasonably accurate nucleation rate estimates and the mislabelling criterion as one giving the relevant cluster size for classical nucleation theory in crystallization studies.

Automated summary

The seeding method is an approximate approach that combines molecular dynamics simulations with classical nucleation theory to study crystallization. By following a mislabelling criterion to select the threshold, consistency between seeding and rigorous methods can be achieved. This work supports the use of seeding for fast and reasonably accurate nucleation rate estimates in crystallization studies.