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Highly stretchable and self-healable supramolecular elastomers are promisingmaterials for future soft electronics, biomimetic systems, and smart textiles,due to their dynamic cross-linking bonds. The dynamic or reversible nature ofthe cross-links gives rise to interesting macroscopic responses in thesematerials such as self-healing and rapid stress-relaxation. However, therelationship between bond activity and macroscopic mechanical response, and theself-healing properties of these dynamic polymer networks (DPNs) remains poorlyunderstood. Using coarse-grained molecular dynamics (CGMD) simulations, wereveal a fundamental connection between the macroscopic behaviors of DPNs andthe shortest paths between distant nodes in the polymer network. Notably, thetrajectories of the material on the shortest path-strain map provide keyinsights into understanding the stress-strain hysteresis, anisotropy, stressrelaxation, and self-healing of DPNs. Based on CGMD simulations under variousloading histories, we formulate a set of empirical rules that dictate how theshortest path interacts with stress and strain. This lays the foundation forthe development of a physics-based theory centered around the non-localmicrostructural feature of shortest paths to predict the mechanical behavior ofDPNs.

Network evolution controlling strain-induced damage and self-healing of elastomers with dynamic bonds