Local Reorientation Dynamics of Semiflexible Polymers in the Melt

Details Local Reorientation Dynamics of Semiflexible Polymers in the Melt Local Reorientation Dynamics of Semiflexible Polymers in the Melt

2000-05-25

arxiv.org/abs/cond-mat/0005432v1

Macromolecules 33(17) 6602-6610 (2000)

Physics

Condensed Matter

Soft Condensed Matter

29 pages, several figures, accepted by Macromolecules

Scientific paper

10.1021/ma000058y

The reorientation dynamics of local tangent vectors of chains in isotropic amorphous melts containing semiflexible model polymers was studied by molecular dynamics simulations. The reorientation is strongly influenced both by the local chain stiffness and by the overall chain length. It takes place by two different subsequent processes: A short-time non-exponential decay and a long-time exponential reorientation arising from the relaxation of medium-size chain segments. Both processes depend on stiffness and chain length. The strong influence of the chain length on the chain dynamics is in marked contrast to its negligible effect on the static structure of the melt. The local structure shows only a small dependence on the stiffness, and is independent of chain length. Calculated correlation functions related to double-quantum NMR experiments are in qualitative agreement with experiments on entangled melts. A plateau is observed in the dependence of segment reorientation on the mean-squared displacement of the corresponding chain segments. This plateau confirms, on one hand, the existence of reptation dynamics. On the other hand, it shows how the reptation picture has to be adapted if, instead of fully flexible chains, semirigid chains are considered.

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