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In recent decades, more than 100 different mechanophores with a broad range of activation forces have been developed. For various applications of mechanophores in polymer materials, it is crucial to selectively activate the mechanophores with high efficiency, avoiding nonspecific bond scission of the material. In this study, we embedded cyclobutane-based mechanophore cross-linkers (I and II) with varied activation forces (fa) in the first network of the double network hydrogels and quantitively investigated the activation selectivity and efficiency of these mechanophores. Our findings revealed that cross-linker I, with a lower activation force relative to the bonds in the polymer main chain (fa-I/fa-chain = 0.8 nN/3.4 nN), achieved efficient activation with 100% selectivity. Conversely, an increase of the activation force of mechanophore II (fa-II/fa-chain = 2.5 nN/3.4 nN) led to a significant decrease of its activation efficiency, accompanied by a substantial number of nonspecific bond scission events. Furthermore, with the coexistence of two cross-linkers, significantly different activation forces resulted in the almost complete suppression of the higher-force one (i.e., I and III, fa-I/fa-III = 0.8 nN/3.4 nN), while similar activation forces led to simultaneous activations with moderate efficiencies (i.e., I and IV, fa-I/fa-IV = 0.8 nN/1.6 nN). These findings provide insights into the prevention of nonspecific bond rupture during mechanophore activation and enhance our understanding of the damage mechanism within polymer networks when using mechanophores as detectors. Besides, it establishes a principle for combining different mechanophores to design multiple mechanoresponsive functional materials. 

Energy dissipation around a propagating crack is the primary mechanism for the enhanced fracture toughness in viscoelastic solids. Such dissipation is spatially non-uniform and is highly coupled to the crack propagation process due to the history-dependent nature of viscoelasticity. We present an experimental approach to map the dissipation field during crack propagation in soft viscoelastic solid. Specifically, we track randomly distributed tracer particles to measure the evolving deformation field. The measured deformation field is then put into a nonlinear constitutive model to determine the dissipation field. Our methodology was used to investigate the deformation and dissipation fields around a propagating crack in a Polyampholyte (PA) hydrogel. The deformation field measurements allowed us to assess whether the commonly assumed translational invariance in viscoelastic fracture theories holds true in practical experiments. Furthermore, by combining the obtained deformation fields with a nonlinear viscoelastic model, we captured the complete history of the dissipation field during crack propagation. We found that dissipation occurred even at material points that are a few millimeters away from the crack tip. The mapped dissipation field also enabled the separate determination of the intrinsic and dissipative components of fracture toughness for the viscoelastic hydrogel. 

When a poroelastic gel is released from a patterned mold, surface stress drives deformation and solvent migration in the gel and flattens its surface profile in a time-dependent manner. Specifically, the gel behaves like an incompressible solid immediately after removal from the mold, and becomes compressible as the solvent is able to squeeze out of the polymer network. In this work, we use the finite element method (FEM) to simulate this transient surface flattening process. We assume that the surface stress is isotropic and constant, the polymer network is linearly elastic and isotropic, and that solvent flow obeys Darcy's law. The short-time and long-time surface profiles can be used to determine the surface stress and drained Poisson's ratio of the gel. Our analysis shows that the drained Poisson's ratio and the diffusivity of the gel can be obtained using interferometry and high-speed video microscopy, without mechanical measurement. 

Double-network gels are a class of tough soft materials comprising two elastic networks with contrasting structures. The formation of a large internal damage zone ahead of the crack tip by the rupturing of the brittle network accounts for the large crack resistance of the materials. Understanding what determines the damage zone is the central question of the fracture mechanics of double-network gels. In this work, we found that at the onset of crack propagation, the size of necking zone, in which the brittle network breaks into fragments and the stretchable network is highly stretched, distinctly decreases with the increase of the solvent viscosity, resulting in a reduction in the fracture toughness of the material. This is in sharp contrast to the tensile behavior of the material that does not change with the solvent viscosity. This result suggests that the dynamics of stretchable network strands, triggered by the rupture of the brittle network, plays a role. To account for this solvent viscosity effect on the crack initiation, a delayed blunting mechanism regarding the polymer dynamics effect is proposed. The discovery on the role of the polymer dynamic adds an important missing piece to the fracture mechanism of this unique material. 

The fracture of highly deformable soft materials is of great practical importance in a wide range of technological applications, emerging in fields such as soft robotics, stretchable electronics, and tissue engineering. From a basic physics perspective, the failure of these materials poses fundamental challenges due to the strongly nonlinear and dissipative deformation involved. In this review, we discuss the physics of cracks in soft materials and highlight two length scales that characterize the strongly nonlinear elastic and dissipation zones near crack tips in such materials. We discuss physical processes, theoretical concepts, and mathematical results that elucidate the nature of the two length scales and show that the two length scales can classify a wide range of materials. The emerging multiscale physical picture outlines the theoretical ingredients required for the development of predictive theories of the fracture of soft materials. We conclude by listing open challenges and directions for future investigations. 

A finite strain nonlinear viscoelastic constitutive model is used to study the uniaxial tension behaviour of chemical polyampholyte (PA) gel. This PA gel is cross-linked by chemical and physical bonds. Our constitutive model attempts to capture the time and strain dependent breaking and healing kinetics of physical bonds. We compare model prediction by uniaxial tension, cyclic and relaxation tests. Material parameters in our model are obtained by least squares optimization. These parameters gave fits that are in good agreement with the experiments.