A numerical model of the partitioning of trace chemical solutes during drop freezing

Partitioning of volatile chemicals among the gas, liquid, and solid phases during freezing of liquid water in clouds can impact trace chemical distributions in the troposphere and in precipitation. We describe here a numerical model of this partitioning during the freezing of a supercooled liquid drop. Our model includes the time-dependent calculation of the coupled processes of crystallization kinetics, heat transport, and solute mass transport, for a freezing hydrometeor particle. We demonstrate the model for tracer partitioning during the freezing of a 1000 μm radius drop on a 100 μm ice substrate, under a few ambient condition scenarios. The model effectively simulates particle freezing and solute transport, yielding results that are qualitatively and quantitatively consistent with previous experimental and theoretical work. Results suggest that the ice shell formation time is governed by heat loss to air and not by dendrite propagation, and that the location of ice nucleation is not important to freezing times or the effective partitioning of chemical solutes. Even for the case of nucleation at the center of the drop, we found that dendrites propagated rapidly to form surface ice. Freezing then proceeded from the outside in. Results also indicate that the solid-liquid interfacial surface area is not important to freezing times or the effective partitioning of chemical solutes, and that the rate aspects of trapping are more important than equilibrium solid-liquid partitioning to the effective partitioning resulting from freezing.