The Effect of Chemistry, Sequence, and Architecture on Complex Coacervation

Complex coacervation is an associative liquid-liquid phase separation phenomenon with a long history of use in a variety of industries, and relevance to new classes of ‘membraneless organelles’ in cells. Coacervate assembly is largely driven by electrostatic attraction coupled with the entropic release of bound counterions and the restructuring of water. We harness model polymer systems to explore the ways in which factors such as the chemical identity (i.e., charge group, polymer backbone chemistry), the patterning or distribution of charges, and the overall size and architecture of the complexing polyelectrolytes modulate the phase behavior of the system. Our experimental efforts are supported by the parallel development of computational approaches to model and predict the phase behavior of coacervate materials. Our goal is to establish molecular-level design rules to facilitate the tailored creation of materials based on complex coacervation that can both illuminate self-assembly phenomena found in nature, and find utility across a wide range of real-world applications.