Molecular Engineering Complex Coacervate Materials Using Sequence

Polyelectrolyte complexation can be used in the self-assembly of a wide range of responsive, bioinspired soft materials. Material responses can include swelling and dissolution or liquid-to-solid transitions, which can be harnessed to facilitate encapsulation and the subsequent fabrication of functional materials. Drawing inspiration from proteins as sequence-controlled polymers, we utilize polypeptides as a model platform to study how the patterning or presentation of charges and other chemical functionalities affects the resulting self-assembly and material properties, including the ability to selectively uptake and stabilize globular proteins. Our experimental efforts are supported by the parallel development of computational approaches for modeling and predicting the phase behavior of patterned polymeric materials. The goal of this systematic investigation is the elucidation of molecular engineering design rules to facilitate the tailored creation of materials based on polyelectrolyte complexation that can both illuminate self-assembly phenomena found in nature, and find utility across a wide range of real-world applications.