Cooperative Dynamics in Unentangled Polymer Fluids

We present a Generalized Langevin Equation for the dynamics of interacting semiflexible polymer chains, undergoing slow cooperative dynamics. The calculated Gaussian intermolecular center-of-mass and monomer potentials, wich enter the GLE, are in quantitative agreement with computer simulation data. The experimentally observed, short-time subdiffusive regime of the polymer mean-square displacements, emerges here from the competition between the intramolecular and the intermolecular mean-force potentials.Comment: 9 pages, latex, 3 figure

Coarse-grained Description of Polymer Blends as Interacting Soft-Colloidal Particles

We present a theoretical approach which maps polymer blends onto mixtures of soft-colloidal particles. The analytical mesoscale pair distribution functions reproduce well data from united atom molecular dynamics simulations of polyolefin mixtures without fitting parameters. The theory exactly recovers the analytical expressions for density and concentration fluctuation structure factors of soft colloidal mixtures (liquid alloys).Comment: 27 REVTex4 pages, 8 PostScript figures, 1 table accepted for publication in Journal of Chemical Physic

Analytical Rescaling of Polymer Dynamics from Mesoscale Simulations

We present a theoretical approach to scale the artificially fast dynamics of simulated coarse-grained polymer liquids down to its realistic value. As coarse-graining affects entropy and dissipation, two factors enter the rescaling: inclusion of intramolecular vibrational degrees of freedom, and rescaling of the friction coefficient. Because our approach is analytical, it is general and transferable. Translational and rotational diffusion of unentangled and entangled polyethylene melts, predicted from mesoscale simulations of coarse-grained polymer melts using our rescaling procedure, are in quantitative agreement with united atom simulations and with experiments.Comment: 6 pages, 2 figures, 2 table

Multiscale Modeling of Binary Polymer Mixtures: Scale Bridging in the Athermal and Thermal Regime

Obtaining a rigorous and reliable method for linking computer simulations of polymer blends and composites at different length scales of interest is a highly desirable goal in soft matter physics. In this paper a multiscale modeling procedure is presented for the efficient calculation of the static structural properties of binary homopolymer blends. The procedure combines computer simulations of polymer chains on two different length scales, using a united atom representation for the finer structure and a highly coarse-grained approach on the meso-scale, where chains are represented as soft colloidal particles interacting through an effective potential. A method for combining the structural information by inverse mapping is discussed, allowing for the efficient calculation of partial correlation functions, which are compared with results from full united atom simulations. The structure of several polymer mixtures is obtained in an efficient manner for several mixtures in the homogeneous region of the phase diagram. The method is then extended to incorporate thermal fluctuations through an effective chi parameter. Since the approach is analytical, it is fully transferable to numerous systems.Comment: in press, 13 pages, 7 figures, 6 table