Microfluidics and Modeling of Nucleation Rates in Cocrystal Systems

Understanding the nucleation process is key to controlling the formation of crystalline materials. Previous studies have demonstrated the potential for static arrays of nanoliter-sized drops to act as miniature reactors that probe the nucleation rate for single component crystals. However, there is little work investigating the nucleation of co-crystal systems. This thesis expands upon drop-based microfluidic strategies to develop a platform that allows for the continuous generation of drops and observe nucleation of crystals within them. The continuous production of drops allows for better scalability, by increasing the number of observable drops without increasing the device size. This experimental approach will eventually allow the nucleation rate to be determined as a function of experimental conditions, including the ratio of co-formers, the coformer concentrations, and the temperature. In addition to the experimental platform, this thesis also contributes to a better understanding of how co-crystal nucleation rates depend on experimental conditions by developing a theoretical model for cocrystal nucleation that is built upon the foundational assumptions of Classical Nucleation Theory. Expanding our understanding of co-crystal nucleation facilitates the construction of time dependent phase diagrams showing how the crystal mixture composition evolves as a result of the nucleation rates. Future work may include using the microfluidic platform to identify new co-crystallizing systems or to determine the polymorphs of previously unexplored crystals.