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Register a new userLinear rheology of reversibly cross-linked biopolymer networks
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We suggest a simple model for reversible cross-links, binding and unbinding to/from a network of semiflexible polymers. The resulting frequency dependent response of the network to an applied shear is calculated via Brownian dynamics simulations. It is shown to be rather complex with the timescale of the linkers competing with the excitations of the network. If the lifetime of the linkers is the longest timescale, as is indeed the case in most biological networks, then a distinct low frequency peak of the loss modulus develops. The storage modulus shows a corresponding decay from its plateau value, which for irreversible cross-linkers extends all the way to the static limit. This additional relaxation mechanism can be controlled by the relative weight of reversible and irreversible linkers.
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Cytoskeletal networks of biopolymers are cross-linked by a variety of proteins. Experiments have shown that dynamic cross-linking with physiological linker proteins leads to complex stress relaxation and enables network flow at long times. We present a model for the mechanical properties of transient networks. By a combination of simulations and analytical techniques we show that a single microscopic timescale for cross-linker unbinding leads to a broad spectrum of macroscopic relaxation times, resulting in a weak power-law dependence of the shear modulus on frequency. By performing rheological experiments, we demonstrate that our model quantitatively describes the frequency behavior of actin network cross-linked with $alpha$-Actinin-$4$ over four decades in frequency.
Starting from a microscopic model of randomly cross-linked particles with quenched disorder, we calculate the Laudau-Wilson free energy S for arbitrary cross-link densities. Considering pure shear deformations, S takes the form of the elastic energy of an isotropic amorphous solid state, from which the shear modulus can be identified. It is found to be an universal quantity, not depending on any microscopic length-scales of the model.
We present a theoretical framework for the linear and nonlinear visco-elastic properties of reversibly crosslinked networks of semiflexible polymers. In contrast to affine models where network strain couples to the polymer end-to-end distance, in our model strain rather serves to locally distort the network structure. This induces bending modes in the polymer filaments, the properties of wich are slaved to the surrounding network structure. Specifically, we investigate the frequency-dependent linear rheology, in particular in combination with crosslink binding/unbinding processes. We also develop schematic extensions to describe the nonlinear response during creep measurements as well as during constant-strainrate ramps.
Reversible crosslinking is a design paradigm for polymeric materials, wherein they are microscopically reinforced with chemical species that form transient crosslinks between the polymer chains. Besides the potential for self-healing, recent experimental work suggests that freely diffusing reversible crosslinks in polymer networks, such as gels, can enhance the toughness of the material without substantial change in elasticity. This presents the opportunity for making highly elastic materials that can be strained to a large extent before rupturing. Here, we employ Gaussian chain theory, molecular simulation, and polymer self-consistent field theory for networks to construct an equilibrium picture for how reversible crosslinks can toughen a polymer network without affecting its linear elasticity. Maximisation of polymer entropy drives the reversible crosslinks to bind preferentially near the permanent crosslinks in the network, leading to local molecular reinforcement without significant alteration of the network topology. In equilibrium conditions, permanent crosslinks share effectively the load with neighbouring reversible crosslinks, forming multi-functional crosslink points. The network is thereby globally toughened, while the linear elasticity is left largely unaltered. Practical guidelines are proposed to optimise this design in experiment, along with a discussion of key kinetic and timescale considerations.
We investigate the system size dependent rheological response of branched type I collagen gels. When subjected to a shear strain, the highly interconnected mesh dynamically reorients, resulting in overall stiffening of the network. When a continuous shear strain is applied to a collagen network, we observe that the local apparent modulus, in the strain-stiffening regime, is strongly dependent on the gel thickness. In addition, we demonstrate that the overall network failure is determined by the ratio of the gel thickness to the mesh size. These findings have broad implications for cell-matrix interactions, the interpretation of rheological tissue data, and the engineering of biomimetic scaffolds.
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