Systematic coarse-graining of the dynamics of entangled polymer melts: the road from chemistry to rheology

Abstract

For optimal processing and design of entangled polymeric materials it is important to establish a rigorous link between the detailed molecular composition of the polymer and the viscoelastic properties of the macroscopic melt. We review current and past computer simulation techniques and critically assess their ability to provide such a link between chemistry and rheology. We distinguish between two classes of coarse-graining levels, which we term coarse-grained molecular dynamics (CGMD) and coarse-grained stochastic dynamics (CGSD). In CGMD the coarse-grained beads are still relatively hard, thus automatically preventing bond crossing. This also implies an upper limit on the number of atoms that can be lumped together and therefore on the longest chain lengths that can be studied. To reach a higher degree of coarse-graining, in CGSD many more atoms are lumped together, leading to relatively soft beads. In that case friction and stochastic forces dominate the interactions, and actions must be undertaken to prevent bond crossing. We also review alternative methods that make use of the tube model of polymer dynamics, by obtaining the entanglement characteristics through a primitive path analysis and by simulation of a primitive chain network. We finally review super-coarse-grained methods in which an entire polymer is represented by a single particle, and comment on ways to include memory effects and transient forces.

Topical review, 31 pages, 10 figures

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• Resolving Dynamic Properties of Polymers through Coarse-Grained Computational Studies
• Dynamics and Rheology of Polymer Melts via Hierarchical Atomistic, Coarse-grained, and Slip-spring Simulations
• On the "generalized Generalized Langevin Equation"
• Information-theoretic tools for parametrized coarse-graining of non-equilibrium extended systems
• Multiscale approach to equilibrating model polymer melts
• Theoretical Reconstruction of Realistic Dynamics of Highly Coarse-Grained cis-1,4-Polybutadiene Melts
• Clustering of entanglement points in highly strained polymer melts
• Crossover Time in Relative Fluctuations Characterizes the Longest Relaxation Time of Entangled Polymers
• Simulation of Entangled Polymer Solutions
• Coarse-Graining of Microscopic Dynamics into Mesoscopic Transient Potential Model
• Application of Projection Operator Method to Coarse-Grained Dynamics with Transient Potential