Aggregation and chimney formation during the solidification of ammonium chloride.

Experiments study large-scale pattern formation during the growth of ammonium chloride (NH4Cl) from solution in a thin (Hele-Shaw) geometry. In particular a solid-liquid mixture ("mushy layer") forms in which growing solid NH4Cl crystals form a solid network interspersed with liquid. There are different ways that the mushy layer can be formed, however. If the cell is heated from below and cooled from above, thermal convection generates large-scale recirculating flows that carry seed crystals from the upper (cold) boundary to the (warmer) side and bottom boundaries. Ballistic deposition of these seed crystals leads to aggregation patterns with significant voids (filled with liquid) with a wide range of length scales. If the cell is cooled from below with a warm environment, the solid NH4Cl grows dendritically without deposition, resulting in a compact mushy layer. Plume convection within this mushy layer produces one or two well-defined "chimneys." If the environment is cool (comparable to the liquidus temperature of the solution), the mushy layer forms by a combination of dendritic growth and ballistic deposition, resulting in a more permeable mushy layer and enhanced chimney formation. The effects of ballistic deposition are enhanced if the cell is tipped, in which case the voids reappear. Plume convection and chimney formation are dramatically enhanced in this case. Additional experiments are done in which fluid flows in the system are enhanced artificially to verify that enhancements in chimney formation are due primarily to the aggregation process, and not to the increases in fluid flows due to thermal and compositional convection.