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  1. 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. 
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    Free, publicly-accessible full text available May 1, 2025
  2. Free, publicly-accessible full text available September 1, 2024
  3. Strong adherence to underwater or wet surfaces for applications like tissue adhesion and underwater robotics is a significant challenge. This is especially apparent when switchable adhesion is required that demands rapid attachment, high adhesive capacity, and easy release. Nature displays a spectrum of permanent to reversible attachment from organisms ranging from the mussel to the octopus, providing inspiration for underwater adhesion design that has yet to be fully leveraged in synthetic systems. Here, we review the challenges and opportunities for creating underwater adhesives with a pathway to switchability. We discuss key material, geometric, modeling, and design tools necessary to achieve underwater adhesion similar to the adhesion control demonstrated in nature. Through these interdisciplinary efforts, we envision that bioinspired adhesives can rise to or even surpass the extraordinary capabilities found in biological systems. 
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    Free, publicly-accessible full text available October 1, 2024
  4. Free, publicly-accessible full text available August 1, 2024
  5. Abstract

    Utilizing colloidal probe, lateral force microscopy and simultaneous confocal microscopy, combined with finite element analysis, we investigate how a microparticle starts moving laterally on a soft, adhesive surface. We find that the surface can form a self-contacting crease at the leading front, which results from a buildup of compressive stress. Experimentally, creases are observed on substrates that exhibit either high or low adhesion when measured in the normal direction, motivating the use of simulations to consider the role of adhesion energy and interfacial strength. Our simulations illustrate that the interfacial strength plays a dominating role in the nucleation of a crease. After the crease forms, it progresses through the contact zone in a Schallamach wave-like fashion. Interestingly, our results suggest that this Schallamach wave-like motion is facilitated by free slip at the adhesive, self-contacting interface within the crease.

     
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  6. Compliant sutures surrounded by stiff matrices are present in biological armors and carapaces, providing enhanced mechanical performance. Understanding the mechanisms through which these sutured composites achieve outstanding properties is key to developing engineering materials with improved strength and toughness. This article studies the impact of suture geometry and load direction on the performance of suture joints using a two-stage reactive polymer resin that enables facile photopatterning of mechanical heterogeneity within a single polymer network. Compliant sinusoidal sutures with varying geometries are photopatterned into stiff matrices, generating a modulus contrast of two orders of magnitude. Empirical relationships are developed connecting suture wavelength and amplitude to composite performance under parallel and perpendicular loading conditions. Results indicate that a greater suture interdigitation broadly improves composite performance when loading is applied perpendicular to suture joints, but has deleterious effects when loading is applied parallel to the joint. Investigations into the failure mechanisms under perpendicular loading highlight the interplay between suture geometry and crack growth stability after damage initiation occurs. Our findings could enable a framework for engineering composites and bio-inspired structures in the future. 
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  7. Chemical recycling of polymers is critical for improving the circular economy of plastics and environmental sustainability. Traditional thermoset polymers have generally been considered permanently crosslinked materials that are difficult or impossible to recycle. Herein, we demonstrate that by activating ‘dormant’ covalent bonds, traditional polycyanurate thermosets can be recycled into the original monomers, which can be circularly reused for their original purpose. Through retrosynthetic analysis, we redirected the synthetic route from forming conventional C–N bonds via irreversible cyanate trimerization to forming the C–O bonds through reversible nucleophilic aromatic substitution of alkoxy-substituted triazine derivatives by alcohol nucleophiles. The new reversible synthetic route enabled the synthesis of previously inaccessible alkyl-polycyanurate thermosets, which exhibit excellent film properties with high chemical resistance, closed-loop recyclability and reprocessing capability. These results show that ‘apparently dormant’ dynamic linkages can be activated and utilized to construct fully recyclable thermoset polymers with a broader monomer scope and increased sustainability. 
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