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Unlike hard materials such as metals and ceramics, rubbery materials canendure large deformations due to the large conformational degree of freedom ofthe crosslinked three-dimensional polymer network. However, the effect of thebranching factor of the network on the ultimate mechanical properties ofrubbery materials has not yet been clarified. This study shows thattri-branching, which entails the lowest branching factor, results in a largeelastic deformation near the theoretical upper bound. This ideal elastic limitis realized by reversible strain-induced crystallization, providing on-demandreinforcement. The findings indicate that the polymer chain is highlyorientated along the stretching axis, whereat enhanced reversiblestrain-induced crystallization is observed in the tri-branched and not in thetetra-branched network. A mathematical theory of structural rigidity is used toexplain the difference in the chain orientation. Although tetra-branchedpolymers have been preferred since the development of vulcanization, thesefindings highlighting the merits of tri-branching will prompt a paradigm shiftin the development of rubbery materials.

Tri-branched gels: Rubbery materials with the lowest branching factor approach the ideal elastic limit