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

J.T. Padding, W.J. Briels

    Research output: Contribution to journalArticleAcademicpeer-review

    74 Citations (Scopus)
    1 Downloads (Pure)

    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 (up to five backbone carbon atoms) 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 (more than ten backbone carbon atoms), leading to relatively soft beads. In that case friction and stochastic forces dominate the interactions, and action 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.
    Original languageEnglish
    Article number233101
    Pages (from-to)233101-1/17
    Number of pages17
    JournalJournal of Physics : Condensed Matter
    Volume23
    DOIs
    Publication statusPublished - 2011

    Fingerprint

    Polymer melts
    Rheology
    rheology
    roads
    chemistry
    Atoms
    Polymers
    polymers
    beads
    atoms
    Molecular dynamics
    Carbon
    molecular dynamics
    carbon
    Chain length
    friction
    computerized simulation
    Friction
    tubes
    Data storage equipment

    Cite this

    @article{1bb6c338d04a4d9f920392d823b3ea2c,
    title = "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 (up to five backbone carbon atoms) 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 (more than ten backbone carbon atoms), leading to relatively soft beads. In that case friction and stochastic forces dominate the interactions, and action 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.",
    author = "J.T. Padding and W.J. Briels",
    year = "2011",
    doi = "10.1088/0953-8984/23/23/233101",
    language = "English",
    volume = "23",
    pages = "233101--1/17",
    journal = "Journal of Physics : Condensed Matter",
    issn = "0953-8984",
    publisher = "Institute of Physics",

    }

    Systematic coarse-graining of the dynamics of entangled polymer melts: the road from chemistry to rheology. / Padding, J.T.; Briels, W.J.

    In: Journal of Physics : Condensed Matter, Vol. 23, 233101, 2011, p. 233101-1/17.

    Research output: Contribution to journalArticleAcademicpeer-review

    TY - JOUR

    T1 - Systematic coarse-graining of the dynamics of entangled polymer melts: the road from chemistry to rheology

    AU - Padding, J.T.

    AU - Briels, W.J.

    PY - 2011

    Y1 - 2011

    N2 - 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 (up to five backbone carbon atoms) 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 (more than ten backbone carbon atoms), leading to relatively soft beads. In that case friction and stochastic forces dominate the interactions, and action 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.

    AB - 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 (up to five backbone carbon atoms) 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 (more than ten backbone carbon atoms), leading to relatively soft beads. In that case friction and stochastic forces dominate the interactions, and action 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.

    U2 - 10.1088/0953-8984/23/23/233101

    DO - 10.1088/0953-8984/23/23/233101

    M3 - Article

    C2 - 21613700

    VL - 23

    SP - 233101-1/17

    JO - Journal of Physics : Condensed Matter

    JF - Journal of Physics : Condensed Matter

    SN - 0953-8984

    M1 - 233101

    ER -