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

Elementary simulation of tethered Brownian motion

We describe a simple numerical simulation, suitable for an undergraduate project (or graduate problem set), of the Brownian motion of a particle in a Hooke-law potential well. Understanding this physical situation is a practical necessity in many experimental contexts, for instance in single molecule biophysics; and its simulation helps the student to appreciate the dynamical character of thermal equilibrium. We show that the simulation succeeds in capturing behavior seen in experimental data on tethered particle motion.Comment: Submitted to American Journal of Physic

Fluctuation-dissipation theorem in an aging colloidal glass

We provide a direct experimental test of the Stokes-Einstein relation as a special case of the fluctuation-dissipation theorem (FDT) in an aging colloidal glass. The use of combined active and passive microrheology allows us to independently measure both the correlation and response functions in this non-equilibrium situation. Contrary to previous reports, we find no deviations from the FDT over several decades in frequency (1 Hz-10 kHz) and for all aging times. In addition, we find two distinct viscoelastic contributions in the aging glass, including a nearly elastic response at low frequencies that grows during aging. This is the clearest change in material properties of the system with aging.Comment: 5 pages,4 figure

Two-point microrheology and the electrostatic analogy

The recent experiments of Crocker et al. suggest that microrheological measurements obtained from the correlated fluctuations of widely-separatedprobe particles determine the rheological properties of soft, complex materials more accurately than do the more traditional particle autocorrelations. This presents an interesting problem in viscoelastic dynamics. We develop an important, simplifing analogy between the present viscoelastic problem and classical electrostatics. Using this analogy and direct calculation we analyze both the one and two particle correlations in a viscoelastic medium in order to explain this observation

One- and two-particle microrheology

We study the dynamics of rigid spheres embedded in viscoelastic media and address two questions of importance to microrheology. First we calculate the complete response to an external force of a single bead in a homogeneous elastic network viscously coupled to an incompressible fluid. From this response function we find the frequency range where the standard assumptions of microrheology are valid. Second we study fluctuations when embedded spheres perturb the media around them and show that mutual fluctuations of two separated spheres provide a more accurate determination of the complex shear modulus than do the fluctuations of a single sphere.Comment: 4 pages, 1 figur

Active Microrheology of Networks Composed of Semiflexible Polymers. II. Theory and comparison with simulations

Building on the results of our computer simulation (ArXiv cond-mat/0503573)we develop a theoretical description of the motion of a bead, embedded in a network of semiflexible polymers, and responding to an applied force. The theory reveals the existence of an osmotic restoring force, generated by the piling up of filaments in front of the moving bead and first deduced through computer simulations. The theory predicts that the bead displacement scales like x ~ t^alfa with time, with alfa=0.5 in an intermediate- and alfa=1 in a long-time regime. It also predicts that the compliance varies with concentration like c^(-4/3) in agreement with experiment.Comment: 18 pages and 2 figure

The response function of a sphere in a viscoelastic two-fluid medium

In order to address basic questions of importance to microrheology, we study the dynamics of a rigid sphere embedded in a model viscoelastic medium consisting of an elastic network permeated by a viscous fluid. We calculate the complete response of a single bead in this medium to an external force and compare the result to the commonly-accepted, generalized Stokes-Einstein relation (GSER). We find that our response function is well approximated by the GSER only within a particular frequency range determined by the material parameters of both the bead and the network. We then discuss the relevance of this result to recent experiments. Finally we discuss the approximations made in our solution of the response function by comparing our results to the exact solution for the response function of a bead in a viscous (Newtonian) fluid.Comment: 12 pages, 2 figure

Nonlinear Elasticity in Biological Gels

Unlike most synthetic materials, biological materials often stiffen as they are deformed. This nonlinear elastic response, critical for the physiological function of some tissues, has been documented since at least the 19th century, but the molecular structure and the design principles responsible for it are unknown. Current models for this response require geometrically complex ordered structures unique to each material. In this Article we show that a much simpler molecular theory accounts for strain stiffening in a wide range of molecularly distinct biopolymer gels formed from purified cytoskeletal and extracellular proteins. This theory shows that systems of semi-flexible chains such as filamentous proteins arranged in an open crosslinked meshwork invariably stiffen at low strains without the need for a specific architecture or multiple elements with different intrinsic stiffnesses.Comment: 23 pages, 5 figures, submitted to Natur