Topologically frustrated dynamics of crowded charged macromolecules in charged hydrogels
Di Jia & Murugappan Muthukumar
Nature Communications volume 9, Article number: 2248 (2018)
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.
Acknowledgements
We thank the National Science Foundation (DMR-1504265), AFOSR Grant FA9550-17-1-0160, and the National Institutes of Health (Grant No. R01HG002776-11) for financial support.
Author information
Affiliations
Department of Polymer Science and Engineering, University of Massachusetts, Amherst, MA, 01003, USA
Di Jia & Murugappan Muthukumar
Contributions
M.M. conceived the project. D.J. designed the experiments, synthesized the gel, and performed all experiments. M.M. developed the theory. Both authors discussed and contributed to the interpretation of the data. The whole project was supervised by M.M.
Competing interests
The authors declare no competing interests.
Corresponding author
Correspondence to Murugappan Muthukumar.
