skip to main content


Title: How chain dynamics affects crack initiation in double-network gels
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.  more » « less
Award ID(s):
1903308
NSF-PAR ID:
10328238
Author(s) / Creator(s):
; ; ; ; ; ; ;
Date Published:
Journal Name:
Proceedings of the National Academy of Sciences
Volume:
118
Issue:
49
ISSN:
0027-8424
Format(s):
Medium: X
Sponsoring Org:
National Science Foundation
More Like this
  1. Toughness of soft materials such as elastomers and gels depends on their ability to dissipate energy and to reduce stress concentration at the crack tip. The primary energy dissipation mechanism is viscoelasticity. Most analyses and models of fracture are based on linear viscoelastic theory (LVT) where strains are assumed to be small and the relaxation mechanisms are independent of stress or strain history. A well-known paradox is that the size of the dissipative zone predicted by LVT is unrealistically small. Here we use a physically based nonlinear viscoelastic model to illustrate why the linear theory breaks down. Using this nonlinear model and analogs of crack problems, we give a plausible resolution to this paradox. In our model, viscoelasticity arises from the breaking and healing of physical cross-links in the polymer network. When the deformation is small, the kinetics of bond breaking and healing are independent of the strain/stress history and the model reduces to the standard linear theory. For large deformations, localized bond breaking damages the material near the crack tip, reducing stress concentration and dissipating energy at the same time. The damage zone size is a new length scale which depends on the strain required to accelerate bond breaking kinetics. These effects are illustrated by considering two cases with stress concentrations: the evolution of spherical damage in a viscoelastic body subjected to internal pressure, and a zero degree peel test. 
    more » « less
  2. Flexible optics and optoelectronic devices require stretchable and compliant antireflection coatings (ARC). Conventional optical coatings, typically inorganic thin films, are brittle and crack under strain, while porous or patterned surfaces often lack environmental endurance and/or involve complex processing. Polymeric optical thin films prepared by initiated chemical vapor deposition (iCVD) comprise a promising alternative class of materials. With iCVD, multilayered, uniform thin film coatings can be synthesized conformally on the surface of a temperature-sensitive substrate near room temperature with precise compositional and thickness control. In this study, a model two-layer coating design consisting of poly(1 H ,1 H ,6 H ,6 H -perfluorohexyl diacrylate) (pPFHDA) with a refractive index at 633 nm of n 633 = 1.426 was deposited atop poly(4-vinylpyridine) (p4VP, n 633 = 1.587). Broadband antireflection over the visible wavelength range (400–750 nm) was conferred to a transparent, flexible thermoplastic polyurethane (TPU) substrate ( n 633 ∼ 1.51), reducing the front-surface reflectance from ∼4% to ∼2%. The superior mechanical compliance of polymer ARCs over conventional inorganic coatings (MgF 2 , SiO 2 , and Al 2 O 3 ) on the TPU substrate was thoroughly investigated by monitoring the evolution of film morphology and tensile fracture with applied equibiaxial strain. The polymer ARC withstood at least ε = 1.64% equibiaxial strain without fracture, while all inorganic coatings cracked. Through a repeated application of strain over hundreds of cycles, the antireflection by the polymer film was shown to possess excellent stability and fatigue resilience. Finally, simulations of established iCVD polymer chemistries possessing larger index contrast revealed that reflectance can be further reduced to <1% or better. 
    more » « less
  3. In materials of all types, hysteresis and toughness are usually correlated. For example, a highly stretchable elastomer or hydrogel of a single polymer network has low hysteresis and low toughness. The single network is commonly toughened by introducing sacrificial bonds, but breaking and possibly reforming the sacrificial bonds causes pronounced hysteresis. In this paper, we describe a principle of stretchable materials that disrupt the toughness–hysteresis correlation, achieving both high toughness and low hysteresis. We demonstrate the principle by fabricating a composite of two constituents: a matrix of low elastic modulus, and fibers of high elastic modulus, with strong adhesion between the matrix and the fibers, but with no sacrificial bonds. Both constituents have low hysteresis (5%) and low toughness (300 J/m2), whereas the composite retains the low hysteresis but achieves high toughness (10,000 J/m2). Both constituents are prone to fatigue fracture, whereas the composite is highly fatigue resistant. We conduct experiment and computation to ascertain that the large modulus contrast alleviates stress concentration at the crack front, and that strong adhesion binds the fibers and the matrix and suppresses sliding between them. Stretchable materials of high toughness and low hysteresis provide opportunities to the creation of high-cycle and low-dissipation soft robots and soft human–machine interfaces.

     
    more » « less
  4. The line crack models, including linear elastic fracture mechanics (LEFM), cohesive crack model (CCM), and extended finite element method (XFEM), rest on the century-old hypothesis of constancy of materials’ fracture energy. However, the type of fracture test presented here, named the gap test, reveals that, in concrete and probably all quasibrittle materials, including coarse-grained ceramics, rocks, stiff foams, fiber composites, wood, and sea ice, the effective mode I fracture energy depends strongly on the crack-parallel normal stress, in-plane or out-of-plane. This stress can double the fracture energy or reduce it to zero. Why hasn’t this been detected earlier? Because the crack-parallel stress in all standard fracture specimens is negligible, and is, anyway, unaccountable by line crack models. To simulate this phenomenon by finite elements (FE), the fracture process zone must have a finite width, and must be characterized by a realistic tensorial softening damage model whose vectorial constitutive law captures oriented mesoscale frictional slip, microcrack opening, and splitting with microbuckling. This is best accomplished by the FE crack band model which, when coupled with microplane model M7, fits the test results satisfactorily. The lattice discrete particle model also works. However, the scalar stress–displacement softening law of CCM and tensorial models with a single-parameter damage law are inadequate. The experiment is proposed as a standard. It represents a simple modification of the three-point-bend test in which both the bending and crack-parallel compression are statically determinate. Finally, a perspective of various far-reaching consequences and limitations of CCM, LEFM, and XFEM is discussed.

     
    more » « less
  5. Understanding how nanoparticles deform under compression is not only of scientific importance, but also has practical significance in various applications such as tribology, nanoparticle-based probes, and dry grinding of raw materials. In this study, we conducted compression tests on model brittle glassy nanoparticles using molecular dynamics simulations. We found that during the early stages of plastic deformation, shear bands formed in a similar pattern regardless of nanoparticle size. However, as the deformation continued, dominant cracks emerged in large nanoparticles while being suppressed in smaller ones. This size-dependent brittle to ductile transition can be explained by a simple model based on Griffith's theory. We also investigated the effect of surface stress state on fracture using thermally tempered nanoparticles. We observed that the presence of compressive surface stress strengthened the nanoparticle by suppressing crack formation, even when a pre-notch was present. On the other hand, tensile surface stress had the opposite effect. Interestingly, nanoparticles with both tensile and compressive surface stress promoted shear deformation, which could potentially compromise the mechanical performance of tempered glass despite delayed crack formation. 
    more » « less