Interfacial friction between semiflexible polymers and crystalline surfaces

The results obtained from molecular dynamics simulations of the friction at an interface between polymer melts and weakly attractive crystalline surfaces are reported. We consider a coarse-grained bead-spring model of linear chains with adjustable intrinsic stiffness. The structure and relaxation dynamics of polymer chains near interfaces are quantified by the radius of gyration and decay of the time autocorrelation function of the first normal mode. We found that the friction coefficient at small slip velocities exhibits a distinct maximum which appears due to shear-induced alignment of semiflexible chain segments in contact with solid walls. At large slip velocities the decay of the friction coefficient is independent of the chain stiffness. The data for the friction coefficient and shear viscosity are used to elucidate main trends in the nonlinear shear rate dependence of the slip length. The influence of chain stiffness on the relationship between the friction coefficient and the structure factor in the first fluid layer is discussed.Comment: 31 pages, 12 figure

Microrheological Characterisation of Anisotropic Materials

We describe the measurement of anisotropic viscoelastic moduli in complex soft materials, such as biopolymer gels, via video particle tracking microrheology of colloid tracer particles. The use of a correlation tensor to find the axes of maximum anisotropy, and hence the mechanical director, is described. The moduli of an aligned DNA gel are reported, as a test of the technique; this may have implications for high DNA concentrations in vivo. We also discuss the errors in microrheological measurement, and describe the use of frequency space filtering to improve displacement resolution, and hence probe these typically high modulus materials.Comment: 5 pages, 5 figures. Replaced after refereeing/ improvement. Main results are the same. The final, published version of the paper is here http://link.aps.org/abstract/PRE/v73/e03190

The relationship between induced fluid structure and boundary slip in nanoscale polymer films

The molecular mechanism of slip at the interface between polymer melts and weakly attractive smooth surfaces is investigated using molecular dynamics simulations. In agreement with our previous studies on slip flow of shear-thinning fluids, it is shown that the slip length passes through a local minimum at low shear rates and then increases rapidly at higher shear rates. We found that at sufficiently high shear rates, the slip flow over atomically flat crystalline surfaces is anisotropic. It is demonstrated numerically that the friction coefficient at the liquid-solid interface (the ratio of viscosity and slip length) undergoes a transition from a constant value to the power-law decay as a function of the slip velocity. The characteristic velocity of the transition correlates well with the diffusion velocity of fluid monomers in the first fluid layer near the solid wall at equilibrium. We also show that in the linear regime, the friction coefficient is well described by a function of a single variable, which is a product of the magnitude of surface-induced peak in the structure factor and the contact density of the adjacent fluid layer. The universal relationship between the friction coefficient and induced fluid structure holds for a number of material parameters of the interface: fluid density, chain length, wall-fluid interaction energy, wall density, lattice type and orientation, thermal or solid walls.Comment: 33 pages, 14 figure

Quantum dot dephasing by edge states

We calculate the dephasing rate of an electron state in a pinched quantum dot, due to Coulomb interactions between the electron in the dot and electrons in a nearby voltage biased ballistic nanostructure. The dephasing is caused by nonequilibrium time fluctuations of the electron density in the nanostructure, which create random electric fields in the dot. As a result, the electron level in the dot fluctuates in time, and the coherent part of the resonant transmission through the dot is suppressed

Gaussian approximation for finitely extensible bead-spring chains with hydrodynamic interaction

The Gaussian Approximation, proposed originally by Ottinger [J. Chem. Phys., 90 (1) : 463-473, 1989] to account for the influence of fluctuations in hydrodynamic interactions in Rouse chains, is adapted here to derive a new mean-field approximation for the FENE spring force. This "FENE-PG" force law approximately accounts for spring-force fluctuations, which are neglected in the widely used FENE-P approximation. The Gaussian Approximation for hydrodynamic interactions is combined with the FENE-P and FENE-PG spring force approximations to obtain approximate models for finitely-extensible bead-spring chains with hydrodynamic interactions. The closed set of ODE's governing the evolution of the second-moments of the configurational probability distribution in the approximate models are used to generate predictions of rheological properties in steady and unsteady shear and uniaxial extensional flows, which are found to be in good agreement with the exact results obtained with Brownian dynamics simulations. In particular, predictions of coil-stretch hysteresis are in quantitative agreement with simulations' results. Additional simplifying diagonalization-of-normal-modes assumptions are found to lead to considerable savings in computation time, without significant loss in accuracy.Comment: 26 pages, 17 figures, 2 tables, 75 numbered equations, 1 appendix with 10 numbered equations Submitted to J. Chem. Phys. on 6 February 200

Evaluating the Applicability of the Fokker-Planck Equation in Polymer Translocation: A Brownian Dynamics Study

Brownian dynamics (BD) simulations are used to study the translocation dynamics of a coarse-grained polymer through a cylindrical nanopore. We consider the case of short polymers, with a polymer length, N, in the range N=21-61. The rate of translocation is controlled by a tunable friction coefficient, gamma_{0p}, for monomers inside the nanopore. In the case of unforced translocation, the mean translocation time scales with polymer length N as ~ (N-N_p)^alpha, where N_p is the average number of monomers in the nanopore. The exponent approaches the value alpha=2 when the pore friction is sufficiently high, in accord with the prediction for the case of the quasi-static regime where pore friction dominates. In the case of forced translocation, the polymer chain is stretched and compressed on the cis and trans sides, respectively, for low gamma_{0p}. However, the chain approaches conformational quasi-equilibrium for sufficiently large gamma_{0p}. In this limit the observed scaling of with driving force and chain length supports the FP prediction that is proportional to N/f_d for sufficiently strong driving force. Monte Carlo simulations are used to calculate translocation free energy functions for the system. The free energies are used with the Fokker-Planck equation to calculate translocation time distributions. At sufficiently high gamma_{0p}, the predicted distributions are in excellent agreement with those calculated from the BD simulations. Thus, the FP equation provides a valid description of translocation dynamics for sufficiently high pore friction for the range of polymer lengths considered here. Increasing N will require a corresponding increase in pore friction to maintain the validity of the FP approach. Outside the regime of low N and high pore friction, the polymer is out of equilibrium, and the FP approach is not valid.Comment: 13 pages, 11 figure

Thermodiffusion in model nanofluids by molecular dynamics simulations

In this work, a new algorithm is proposed to compute single particle (infinite dilution) thermodiffusion using Non-Equilibrium Molecular Dynamics simulations through the estimation of the thermophoretic force that applies on a solute particle. This scheme is shown to provide consistent results for simple Lennard-Jones fluids and for model nanofluids (spherical non-metallic nanoparticles + Lennard-Jones fluid) where it appears that thermodiffusion amplitude, as well as thermal conductivity, decrease with nanoparticles concentration. Then, in nanofluids in the liquid state, by changing the nature of the nanoparticle (size, mass and internal stiffness) and of the solvent (quality and viscosity) various trends are exhibited. In all cases the single particle thermodiffusion is positive, i.e. the nanoparticle tends to migrate toward the cold area. The single particle thermal diffusion 2 coefficient is shown to be independent of the size of the nanoparticle (diameter of 0.8 to 4 nm), whereas it increases with the quality of the solvent and is inversely proportional to the viscosity of the fluid. In addition, this coefficient is shown to be independent of the mass of the nanoparticle and to increase with the stiffness of the nanoparticle internal bonds. Besides, for these configurations, the mass diffusion coefficient behavior appears to be consistent with a Stokes-Einstein like law

XMM-Newton and INTEGRAL analysis of the Supergiant Fast X-ray Transient IGR J17354-3255

We present the results of combined INTEGRAL and XMM-Newton observations of the supergiant fast X-ray transient (SFXT) IGR J17354$-$3255. Three XMM-Newton observations of lengths 33.4 ks, 32.5 ks and 21.9 ks were undertaken, the first an initial pointing to identify the correct source in the field of view and the latter two performed around periastron. Simultaneous INTEGRAL observations across $\sim66\%$ of the orbital cycle were analysed but the source was neither detected by IBIS/ISGRI nor by JEM-X. The XMM-Newton light curves display a range of moderately bright X-ray activity but there are no particularly strong flares or outbursts in any of the three observations. We show that the spectral shape measured by XMM-Newton can be fitted by a consistent model throughout the observation, suggesting that the observed flux variations are driven by obscuration from a wind of varying density rather than changes in accretion mode. The simultaneous INTEGRAL data rule out simple extrapolation of the simple powerlaw model beyond the XMM-Newton energy range.Comment: 13 pages, 9 figures, This article has been accepted for publication in Monthly Notices of the Royal Astronomical Society Published by Oxford University Pres

Signature of elasticity in the Faraday instability

We investigate the onset of the Faraday instability in a vertically vibrated wormlike micelle solution. In this strongly viscoelastic fluid, the critical acceleration and wavenumber are shown to present oscillations as a function of driving frequency and fluid height. This effect, unseen neither in simple fluids nor in previous experiments on polymeric fluids, is interpreted in terms of standing elastic waves between the disturbed surface and the container bottom. It is shown that the model of S. Kumar [Phys. Rev. E, {\bf 65}, 026305 (2002)] for a viscoelastic fluid accounts qualitatively for our experimental observations. Explanations for quantitative discrepancies are proposed, such as the influence of the nonlinear rheological behaviour of this complex fluid.Comment: 4 pages, 4 figure

Parallel Temperatures in Supersonic Beams: Ultra Cooling of Light Atoms seeded in a Heavier Carrier Gas

We have found recently that, in a supersonic expansion of a mixture of two monoatomic gases, the parallel temperatures of the two gases can be very different. This effect is large if the seeded gas is highly diluted and if its atomic mass is considerably smaller than the one of the carrier gas. In the present paper, we present a complete derivation of our theoretical analysis of this effect. Our calculation is a natural extension of the existing theory of supersonic cooling to the case of a gas mixture, in the high dilution limit. Finally, we describe a set of temperature measurements made on a beam of lithium seeded in argon. Our experimental results are in very good agreement with the results of our calculation.Comment: 24 novembre 200