Determining Microscopic Viscoelasticity in Flexible and Semiflexible Polymer Networks from Thermal Fluctuations

We have developed a new technique to measure viscoelasticity in soft materials such as polymer solutions, by monitoring thermal fluctuations of embedded probe particles using laser interferometry in a microscope. Interferometry allows us to obtain power spectra of fluctuating beads from 0.1 Hz to 20 kHz, and with sub-nanometer spatial resolution. Using linear response theory, we determined the frequency-dependent loss and storage shear moduli up to frequencies on the order of a kHz. Our technique measures local values of the viscoelastic response, without actively straining the system, and is especially suited to soft biopolymer networks. We studied semiflexible F-actin solutions and, as a control, flexible polyacrylamide (PAAm) gels, the latter close to their gelation threshold. With small particles, we could probe the transition from macroscopic viscoelasticity to more complex microscopic dynamics. In the macroscopic limit we find shear moduli at 0.1 Hz of G'=0.11 +/- 0.03 Pa and 0.17 +/- 0.07 Pa for 1 and 2 mg/ml actin solutions, close to the onset of the elastic plateau, and scaling behavior consistent with G(omega) as omega^(3/4) at higher frequencies. For polyacrylamide we measured plateau moduli of 2.0, 24, 100 and 280 Pa for crosslinked gels of 2, 2.5, 3 and 5% concentration (weight/volume) respectively, in agreement to within a factor of two with values obtained from conventional rheology. We also found evidence for scaling of G(omega) as \omega^(1/2), consistent with the predictions of the Rouse model for flexible polymers.Comment: 16 pages, with 15 PostScript figures (to be published in Macromolecules

Instability and front propagation in laser-tweezed lipid bilayer tubules

We study the mechanism of the `pearling' instability seen recently in experiments on lipid tubules under a local applied laser intensity. We argue that the correct boundary conditions are fixed chemical potentials, or surface tensions \Sigma, at the laser spot and the reservoir in contact with the tubule. We support this with a microscopic picture which includes the intensity profile of the laser beam, and show how this leads to a steady-state flow of lipid along the surface and gradients in the local lipid concentration and surface tension (or chemical potential). This leads to a natural explanation for front propagation and makes several predictions based on the tubule length. While most of the qualitative conclusions of previous studies remain the same, the `ramped' control parameter (surface tension) implies several new qualitative results. We also explore some of the consequences of front propagation into a noisy (due to pre-existing thermal fluctuations) unstable medium.Comment: 12 page latex + figures using epsf.sty to be published in Journal de Physique II, January 199

Effective medium approach for stiff polymer networks with flexible cross-links

Recent experiments have demonstrated that the nonlinear elasticity of in vitro networks of the biopolymer actin is dramatically altered in the presence of a flexible cross-linker such as the abundant cytoskeletal protein filamin. The basic principles of such networks remain poorly understood. Here we describe an effective medium theory of flexibly cross-linked stiff polymer networks. We argue that the response of the cross-links can be fully attributed to entropic stiffening, while softening due to domain unfolding can be ignored. The network is modeled as a collection of randomly oriented rods connected by flexible cross-links to an elastic continuum. This effective medium is treated in a linear elastic limit as well as in a more general framework, in which the medium self-consistently represents the nonlinear network behavior. This model predicts that the nonlinear elastic response sets in at strains proportional to cross-linker length and inversely proportional to filament length. Furthermore, we find that the differential modulus scales linearly with the stress in the stiffening regime. These results are in excellent agreement with bulk rheology data.Comment: 12 pages, 8 figure

Origin of slow stress relaxation in the cytoskeleton

Dynamically crosslinked semiflexible biopolymers such as the actin cytoskeleton govern the mechanical behavior of living cells. Semiflexible biopolymers nonlinearly stiffen in response to mechanical loads, whereas the crosslinker dynamics allow for stress relaxation over time. Here we show, through rheology and theoretical modeling, that the combined nonlinearity in time and stress leads to an unexpectedly slow stress relaxation, similar to the dynamics of disordered systems close to the glass transition. Our work suggests that transient crosslinking combined with internal stress can explain prior reports of soft glassy rheology of cells, in which the shear modulus increases weakly with frequency.Comment: 6 pages, 4 figure

Deformation of crosslinked semiflexible polymer networks

Networks of filamentous proteins play a crucial role in cell mechanics. These cytoskeletal networks, together with various crosslinking and other associated proteins largely determine the (visco)elastic response of cells. In this letter we study a model system of crosslinked, stiff filaments in order to explore the connection between the microstructure under strain and the macroscopic response of cytoskeletal networks. We find two distinct regimes as a function primarily of crosslink density and filament rigidity: one characterized by affine deformation and one by non-affine deformation. We characterize the crossover between these two.Comment: Typos fixed and some technical details clarified. To appear in Phys. Rev. Let

Criticality and isostaticity in fiber networks

The rigidity of elastic networks depends sensitively on their internal connectivity and the nature of the interactions between constituents. Particles interacting via central forces undergo a zero-temperature rigidity-percolation transition near the isostatic threshold, where the constraints and internal degrees of freedom are equal in number. Fibrous networks, such as those that form the cellular cytoskeleton, become rigid at a lower threshold due to additional bending constraints. However, the degree to which bending governs network mechanics remains a subject of considerable debate. We study disordered fibrous networks with variable coordination number, both above and below the central-force isostatic point. This point controls a broad crossover from stretching- to bending-dominated elasticity. Strikingly, this crossover exhibits an anomalous power-law dependence of the shear modulus on both stretching and bending rigidities. At the central-force isostatic point---well above the rigidity threshold---we find divergent strain fluctuations together with a divergent correlation length $\xi$, implying a breakdown of continuum elasticity in this simple mechanical system on length scales less than $\xi$.Comment: 6 pages, 5 figure

Elastic response of filamentous networks with compliant crosslinks

Experiments have shown that elasticity of disordered filamentous networks with compliant crosslinks is very different from networks with rigid crosslinks. Here, we model and analyze filamentous networks as a collection of randomly oriented rigid filaments connected to each other by flexible crosslinks that are modeled as worm-like chains. For relatively large extensions we allow for enthalpic stretching of crosslinks' backbones. We show that for sufficiently high crosslink density, the network linear elastic response is affine on the scale of the filaments' length. The nonlinear regime can become highly nonaffine and is characterized by a divergence of the elastic modulus at finite strain. In contrast to the prior predictions, we do not find an asymptotic regime in which the differential elastic modulus scales linearly with the stress, although an approximate linear dependence can be seen in a transition from entropic to enthalpic regimes. We discuss our results in light of the recent experiments.Comment: 10 pages, 11 figure

Non-equilibrium mechanics and dynamics of motor activated gels

The mechanics of cells is strongly affected by molecular motors that generate forces in the cellular cytoskeleton. We develop a model for cytoskeletal networks driven out of equilibrium by molecular motors exerting transient contractile stresses. Using this model we show how motor activity can dramatically increase the network's bulk elastic moduli. We also show how motor binding kinetics naturally leads to enhanced low-frequency stress fluctuations that result in non-equilibrium diffusive motion within an elastic network, as seen in recent \emph{in vitro} and \emph{in vivo} experiments.Comment: 21 pages, 8 figure