Structural and mechanical analysis of H-bonding functionalized bottlebrush melts and networks

Brush hydrogels are synthetically produced materials with desirable variability in parameters such as softness and firmness, which can be tuned by varying grafting density and length of side chains. While the persistence length of the bottlebrushes in such a system can be effectively changed through this tuning as well, it is not applicable for most biomedical applications. Experimentally, it has been observed that H-bonding interactions between side chains produce well-defined helices in the backbones of certain bottlebrush polymers, implying that bottlebrush polymers with functionalized side chains can produce repeating structures that are resistant to thermal fluctuations. Through a coarse-grained approach, we have been able to form a qualitatively well-defined helix in the backbone of a single bottlebrush polymer with charged sites mimicking H-bonding. In extending this to polymer melt and crosslinked polymer systems, we have been able to observe that the structures of these bottlebrushes' backbones are preserved by crosslinking and inter-chain interactions between the side chains of different brushes. We now seek to quantify these relationships through trajectory analysis under different temperature and dielectric annealing conditions.