Abstract
Extracellular matrices composed of filamentous biopolymers like collagen and fibrin have viscoelastic properties that differ from those of rubberlike elastomers or hydrogels formed by flexible polymers. Compared to flexible polymer gels, filamentous biopolymer networks generally have larger elastic moduli, a striking increase in elastic modulus with increasing strain, and a pronounced negative normal stress when deformed in simple shear. All three of these unusual features can be accounted for by a theory that extends concepts of entropic elasticity to a regime where the polymer chains are already significantly extended in the absence of external forces because of their finite bending stiffness. An essential assumption of the theories that relate microscopic structural parameters such as persistence length and mesh size of biopolymer gels to their macroscopic rheology is that the deformation of these materials is affine: that is, the macroscopic strain of the bulk material is equal to the local strain within the material at each point. The validity of this assumption for the dilute open meshworks of most biopolymer gels has been experimentally tested by embedding micron diameter fluorescent beads within the networks formed by fibrin and quantifying their displacements as the macroscopic samples are deformed in a rheometer. Measures of non-affine deformation are small at small strains and decrease as strain increases and the sample stiffens. These results are consistent with the entropic model for non-linear elasticity of semiflexible polymer networks and show that strain-stiffening does not require non-affine deformations.
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