An extreme toughening mechanism for soft materials.

Soft yet tough materials are ubiquitous in nature and everyday life. The ratio between fracture toughness and intrinsic fracture energy of a soft material defines its toughness enhancement. Soft materials' toughness enhancement has been long attributed to their bulk stress-stretch hysteresis induced by dissipation mechanisms such as Mullins effect and viscoelasticity. With a combination of experiments and theory, here we show that the bulk dissipation mechanisms significantly underestimate the toughness enhancement of soft tough materials. We propose a new mechanism and scaling law to account for extreme toughening of diverse soft materials. We show that the toughness enhancement of soft materials relies on both bulk hysteretic dissipation, and near-crack dissipation due to mechanisms such as polymer-chain entanglement. Unlike the bulk hysteretic dissipation, the near-crack dissipation does not necessarily induce large stress-stretch hysteresis of the bulk material. The extreme toughening mechanism can be potentially universally applied to various soft tough materials, ranging from double-network hydrogels, interpenetrating-network hydrogels, entangled-network hydrogels and slide-ring hydrogels, to unfilled and filled rubbers.