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Register a new userThe effect of chain polydispersity on the elasticity of disordered polymer networks
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Due to their unique structural and mechanical properties, randomly-crosslinked polymer networks play an important role in many different fields, ranging from cellular biology to industrial processes. In order to elucidate how these properties are controlled by the physical details of the network (textit{e.g.} chain-length and end-to-end distributions), we generate disordered phantom networks with different crosslinker concentrations $C$ and initial density $rho_{rm init}$ and evaluate their elastic properties. We find that the shear modulus computed at the same strand concentration for networks with the same $C$, which determines the number of chains and the chain-length distribution, depends strongly on the preparation protocol of the network, here controlled by $rho_{rm init}$. We rationalise this dependence by employing a generic stress-strain relation for polymer networks that does not rely on the specific form of the polymer end-to-end distance distribution. We find that the shear modulus of the networks is a non-monotonic function of the density of elastically-active strands, and that this behaviour has a purely entropic origin. Our results show that if short chains are abundant, as it is always the case for randomly-crosslinked polymer networks, the knowledge of the exact chain conformation distribution is essential for predicting correctly the elastic properties. Finally, we apply our theoretical approach to published experimental data, qualitatively confirming our interpretations.
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Disordered biopolymer gels have striking mechanical properties including strong nonlinearities. In the case of athermal gels (such as collagen-I) the nonlinearity has long been associated with a crossover from a bending dominated to a stretching dominated regime of elasticity. The physics of this crossover is related to the existence of a central-force isostatic point and to the fact that for most gels the bending modulus is small. This crossover induces scaling behavior for the elastic moduli. In particular, for linear elasticity such a scaling law has been demonstrated [Broedersz et al. Nature Physics, 2011 7, 983]. In this work we generalize the scaling to the nonlinear regime with a two-parameter scaling law involving three critical exponents. We test the scaling law numerically for two disordered lattice models, and find a good scaling collapse for the shear modulus in both the linear and nonlinear regimes. We compute all the critical exponents for the two lattice models and discuss the applicability of our results to real systems.
The modeling of the elastic properties of disordered or nanoscale solids requires the foundations of the theory of elasticity to be revisited, as one explores scales at which this theory may no longer hold. The only cases for which microscopically based derivations of elasticity are documented are (nearly) uniformly strained lattices. A microscopic approach to elasticity is proposed. As a first step, microscopically exact expressions for the displacement, strain and stress fields are derived. Conditions under which linear elastic constitutive relations hold are studied theoretically and numerically. It turns out that standard continuum elasticity is not self-evident, and applies only above certain spatial scales, which depend on details of the considered system and boundary conditions. Possible relevance to granular materials is briefly discussed.
We study the shape, elasticity and fluctuations of the recently predicted (cond-mat/9510172) and subsequently observed (in numerical simulations) (cond-mat/9705059) tubule phase of anisotropic membranes, as well as the phase transitions into and out of it. This novel phase lies between the previously predicted flat and crumpled phases, both in temperature and in its physical properties: it is crumpled in one direction, and extended in the other. Its shape and elastic properties are characterized by a radius of gyration exponent $ u$ and an anisotropy exponent $z$. We derive scaling laws for the radius of gyration $R_G(L_perp,L_y)$ (i.e. the average thickness) of the tubule about a spontaneously selected straight axis and for the tubule undulations $h_{rms}(L_perp,L_y)$ transverse to its average extension. For phantom (i.e. non-self-avoiding) membranes, we predict $ u=1/4$, $z=1/2$ and $eta_kappa=0$, exactly, in excellent agreement with simulations. For membranes embedded in the space of dimension $d<11$, self-avoidance greatly swells the tubule and suppresses its wild transverse undulations, changing its shape exponents $ u$ and $z$. We give detailed scaling results for the shape of the tubule of an arbitrary aspect ratio and compute a variety of correlation functions, as well as the anomalous elasticity of the tubules. Finally we present a scaling theory for the shape of the membrane and its specific heat near the continuous transitions into and out of the tubule phase and perform detailed renormalization group calculations for the crumpled-to-tubule transition for phantom membranes.
The onset of rigidity in interacting liquids, as they undergo a transition to a disordered solid, is associated with a dramatic rearrangement of the low-frequency vibrational spectrum. In this letter, we derive scaling forms for the singular dynamical response of disordered viscoelastic networks near both jamming and rigidity percolation. Using effective-medium theory, we extract critical exponents, invariant scaling combinations and analytical formulas for universal scaling functions near these transitions. Our scaling forms describe the behavior in space and time near the various onsets of rigidity, for rigid and floppy phases and the crossover region, including diverging length and time scales at the transitions. We expect that these behaviors can be measured in systems ranging from colloidal suspensions to anomalous charge-density fluctuations of strange metals.
We study the phenomenon of migration of the small molecular weight component of a binary polymer mixture to the free surface using mean field and self-consistent field theories. By proposing a free energy functional that incorporates polymer-matrix elasticity explicitly, we compute the migrant volume fraction and show that it decreases significantly as the sample rigidity is increased. Estimated values of the bulk modulus suggest that the effect should be observable experimentally for rubber-like materials. This provides a simple way of controlling surface migration in polymer mixtures and can play an important role in industrial formulations, where surface migration often leads to decreased product functionality.
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