Exploiting supramolecular associations in interpenetrating networks and elastomers*

Supramolecular interactions may hold the key to the development of network systems with tunable mechanics and modulated architecture, such as observed in the muscle protein titin. It is the dynamic nature of these physical associations that we have exploited in the design of tough supramolecular materials that super-impose covalent and non-covalent interactions to tailor tensile response. We have developed supramolecular elastomers and interpenetrating network (IPN) systems that probe the interplay of non-covalent and covalent interactions in structural organization and mechanical response. By tailoring physical associations via control of self-assembly and composition, we have demonstrated enhanced supramolecular dynamics driven by architecture and toughness enhancements due to phase behavior. Recently, non-covalent interaction strength, network regularity, and chemoresponsiveness have been utilized as handles to derive gradient materials and to induce actuation behavior.