Abstract
Unlike hard materials such as metals and ceramics, rubbery materials can endure large deformations due to the large conformational degree of freedom of the cross-linked polymer network. However, the effect of the network's branching factor on the ultimate mechanical properties has not yet been clarified. This study shows that tri-branching, which entails the lowest branching factor, results in a large elastic deformation near the theoretical upper bound. This ideal elastic limit is realized by reversible strain-induced crystallization, providing on-demand reinforcement. The enhanced reversible strain-induced crystallization is observed in the tri-branched and not in the tetra-branched network. A mathematical theory of structural rigidity is used to explain the difference in the chain orientation. Although tetra-branched polymers have been preferred since the development of vulcanization, these findings highlighting the merits of tri-branching will prompt a paradigm shift in the development of rubbery materials.