Microrheology of biopolymer-membrane complexes

We create tailored microstructures, consisting of complexes of lipid membranes with self-assembled biopolymer shells, to study the fundamental properties and interactions of these basic components of living cells. We measure the mechanical response of these artificial structures at the micrometer scale, using optical tweezers and single-particle tracking. These systems exhibit rich dynamics that illustrate the viscoelastic character of the quasi-two-dimensional biopolymer network. We present a theoretical model relating the rheological properties of these membranes to the observed dynamics.     

Structure and dynamics of a polymer melt at an attractive surface

We study the structural and dynamic properties of a polymer melt in the vicinity of an adhesive solid substrate by means of Molecular Dynamics simulation at various degrees of surface adhesion. The properties of the individual polymer chains are examined as a function of the distance to the interface and found to agree favorably with theoretical predictions. Thus, the adsorbed amount at the adhesive surface is found to scale with the macromolecule length as $\Gamma \propto \sqrt N$ , regardless of the adsorption strength. For chains within the range of adsorption we analyze in detail the probability size distributions of the various building blocks: loops, tails and trains, and find that loops and tails sizes follow power laws while train lengths decay exponentially thus confirming some recent theoretical results. The chain dynamics as well as the monomer mobility are also investigated and found to depend significantly on the proximity of a given layer to the solid adhesive surface with onset of vitrification for sufficiently strong adsorption.      

Microrheology of entangled F-actin solutions

We measure the viscoelasticity of entangled F-actin over length scales between 1 and 100 microm using one- and two-particle microrheology, and directly identify two distinct microscopic contributions to the elasticity. Filament entanglements lead to a frequency-independent elastic modulus over an extended frequency range of 0.01-30 rad/sec; this is probed with one-particle microrheology. Longitudinal fluctuations of the filaments increase the elastic modulus between 0.1 and 30 rad/sec at length scales up to the filament persistence length; this is probed by two-particle microrheology.     

Instantons and representations of an associative algebra

We give the correspondence between instantons onS ⁴ and some representations of an associative algebra. For the given structure group, we get simultaneous imbeddings to (the inductive limit) of the moduli spaces for instantons onS ⁴ of all instanton numbers.     

Equilibrium dynamics in the nondiffusive regime of an entangled polymer blend

The dynamics of compositional fluctuations in a miscible, entangled homopolymer blend of poly(ethylene oxide) and poly(methyl methacrylate) were studied on length scales smaller than the polymer radii of gyration, and for times comparable to the polymers' disentanglement time. The measured relaxation rates are consistent with predictions of the reptation model, as expressed via the dynamic random-phase approximation. Moreover, the observed mode amplitudes allow for an estimate of the entanglement length in the blend.     

Collective dynamics of an end-grafted polymer brush in solvents of varying quality

The dynamic structure of a chemically end-grafted polystyrene brush bathed in solvents of varying interactions was studied by evanescent wave dynamic light scattering. It reveals distinct behavior under good and poor solvent conditions. The cooperative diffusion is a generic feature of a good solvent environment, whereas a second slow relaxation mode appears in the theta solvent regime. Its characteristics resemble self-diffusion of clusters in a gel while weak concentration fluctuations in the polymer brush decay similarly to a semidilute polymer solution.     

Turbulent dynamics of polymer solutions

We study properties of dilute polymer solutions. The probability density function (PDF) of polymer end-to-end extensions R in turbulent flows is examined. We show that if the value of the Lyapunov exponent lambda is smaller than the inverse molecular relaxation time 1/tau then the PDF has a strong peak at the equilibrium size R0 and a power tail at R>R0. This confirms and extends the results of J. L. Lumley [Symp. Math. 9, 315 (1972)]. There is no essential influence of polymers on the flow in this regime. At lambdatau>1 the majority of molecules is stretched to the linear size R(op)>R0, which can be much smaller than the maximal length of the molecules due to their back reaction.     

Surface dynamics of polymer films

The dynamics of supported polymer films were studied by probing the surface height fluctuations as a function of lateral length scale using x-ray photon correlation spectroscopy. Measurements were performed on polystyrene (PS) films of thicknesses varying from 84 to 333 nm at temperatures above the PS glass transition temperature. Within a range of wave vectors spanning 10(-3) to 10(-2) nm(-1), good agreement is found between the measured surface dynamics and the theory of overdamped thermal capillary waves on thin films. Quantitatively, the data can be accounted for using the viscosity of bulk PS.     

Effective temperature scaled dynamics of a flexible polymer in an active bath

Langevin dynamics simulations are employed to study the dynamical properties of a flexible polymer in an active bath. The diffusion of the centre of mass and end-to-end distance fluctuation are particularly analysed. We modulate both active force and active particle size to probe the activity-induced facilitation of polymer dynamics. Results indicate diffusivity and chain relaxation time can be well scaled by the effective temperature of the active bath. In addition, diffusion dynamics demonstrates an anomalous superdiffusive behaviour in short time scales, which becomes more prominent with increasing active particle size. Lastly, we extract the effective viscosity experienced by the probed chain, showing a sharp decrease with increment of effective temperature. The attenuation of effective viscosity due to activity might be responsible for the facilitated polymer dynamics.     

Microrheology from rotational diffusion of colloidal particles

The microrheology of viscoelastic fluids is obtained from rotational diffusion of optically anisotropic spherical colloidal probes, measured by depolarized dynamic light scattering. The storage and loss moduli obtained from the rotational mean squared displacement is in excellent agreement with those obtained from translational diffusion and by mechanical measurements. We also show that this method is applicable to samples with strong light scattering components. This extends the capabilities of the microrheological methods based on the diffusional motion of colloidal probes.     

Microrheology of the liquid-solid transition during gelation

The viscoelastic properties of physical and chemical polymer gels are characterized through the liquid-solid transition using particle tracking microrheology. Measurements of the probe particle mean-squared displacement are shifted as the extent of gelation increases to generate master curves. From the shift factors, we determine the gel point and critical scaling exponents. Both systems exhibit a critical relaxation exponent n approximately 0.6, where G' approximately G' approximately omega n for the incipient gel, consistent with the Rouse model of dynamic scaling in the percolation universality class.     

Theory of the dynamics of the Hopfield model of associative memory

We present an analysis of the parallel dynamics of the Hopfield model of the associative memory of a neural network without recourse to the replica formalism. A probabilistic method based on the signal-to-noise ratio is employed to obtain a simple recursion relation for the zero temperature as well as the finite temperature dynamics of the network. The fixed points of the recursion relation and their basins of attraction are found to be in fairly satisfactory agreement with the numerical simulations of the model. We also present some new numerical results which support our recursion relation and throw light on the nature of the ensemble of the network states which are optimized with respect to single spin flips.     

Tube theory of entangled polymer dynamics

The dynamics of entangled flexible polymers is dominated by physics general to many chemical systems. It is an appealing interdisciplinary field where experimental and theoretical physics can work closely with chemistry and chemical engineering. The role of topological interactions is particularly important, and has given rise to a successful theoretical framework: the 'tube model'. Progress over the last 30 years is reviewed in the light of specially-synthesized model materials, an increasing palette of experimental techniques, simulation and both linear and nonlinear rheological response. Our current understanding of a series of processes in entangled dynamics: 'reptation', 'contour length fluctuation' and 'constraint-release' are set in the context of remaining serious challenges. Especial attention is paid to the phenomena associated with polymers of complex topology or 'long chain branching'.     

Viscoelastic dynamics of polymer thin films and surfaces

The strain relaxation behavior in a viscoelastic material, such as a polymer melt, may be strongly affected by the proximity of a free surface or mobile interface. In this paper, the viscoelastic surface modes of the material are discussed with respect to their possible influence on the freezing temperature and dewetting morphology of thin polymer films. In particular, the mode spectrum is connected with mode coupling theory assuming memory effects in the melt. Based on the idea that the polymer freezes due to these memory effects, surface melting is predicted. As a consequence, the substantial shift of the glass transition temperature of thin polymer films with respect to the bulk is naturally explanied. The experimental findings of several independent groups can be accounted for quantitatively, with the elastic modulus at the glass transition temperature as the only fitting parameter. Finally, a simple model is put forward which accounts for the occurrence of certain generic dewetting morphologies in thin liquid polymer films. It demonstrates that by taking into account the viscoelastic properties of the film, a morphological phase diagram may be derived which describes the observed structures of dewetting fronts. It is demonstrated that dewetting morphologies may also serve to determine nanoscale rheological properties of liquids.Received: 1 January 2003, Published online: 14 October 2003PACS: 47.50. + d Non-Newtonian fluid flows - 68.47.Mn Polymer surfaces - 68.60.Dv Thermal stability; thermal effects     

Multiple scattering and scaling in dynamics of polymer solutions

A new stochastic model for describing polymer dynamics in solutions at finite concentration is presented. When a multiple-scattering formalism is incorporated, there emerge the coupled equations which areisomorphic to the Freed-Edwards theory. Various scaling properties are shown to be contained therein.     

Laser-induced ablation dynamics and flight of thin polymer films

We investigated the ejection dynamics of triazene polymer layers in the thickness range of 40 nm to 600 nm upon nanosecond laser ablation at a wavelength of 532 nm. The ablation is due to laser-induced thermal degradation of a small part of the polymer in contact with the silicon substrate. The subsequent dynamics of the flying polymer layer are measured with sub-nanosecond time resolution. The evaluation of the initial velocity for different film thicknesses gives insight into the energy transfer process during the acceleration of the films.