Topologically frustrated dynamics of crowded charged macromolecules in charged hydrogels

Abstract

Movement of charged macromolecules in crowded aqueous environments is a ubiquitous phenomenon vital to the various living processes and formulations of materials for health care. While study of diffusion of tracer amounts of probe macromolecules trapped inside concentrated solutions, gels, or random media has led to an enhanced understanding of this complex process, the collective dynamics of charged macromolecules embedded inside congested charge-bearing matrices still remains to be fully explored. Here we report a frustrated dynamics of DNA and synthetic polyelectrolytes inside a charged host hydrogel where the guest molecules do not diffuse. Instead, they exhibit a family of relaxation processes arising from a combination of conformational entropy and local chain dynamics, which are frustrated by the confinement from the gel. We also have developed a model explaining this new universality class of non-diffusive topologically frustrated dynamics of charged macromolecules.