Mode-mode-coupling theory of the dynamics of polymeric liquids

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Abstract

A first principles, statistical mechanical theory of the dynamics of polymer liquids has been developed using the generalized Langevin equation and molecular-scale mode-mode-coupling methods. The essential physics of chain uncrossability and connectivity is contained in a time-dependent dynamical friction matrix, which quantitatively described fluctuating force correlations and many-body caging. For very long chain fluids, the predicted molecular weight dependences of the transport coefficients agree qualitatively with the reptation/tube theory. However, a more general physical interpretation appears to exist, and a natural analogy with critical slowing down is suggested. Polymer shape fluctuation effects are also included in a microscopic fashion, and when dominant generate both a stretched exponential terminal relaxation and a 3.55 exponent for the viscosity-chain-length scaling law. Anomalous segmental and center-of-mass diffusion at early times are also studied.

Original languageEnglish (US)
Pages (from-to)643-649
Number of pages7
JournalJournal of Non-Crystalline Solids
Volume131-133
Issue numberPART 2
DOIs
StatePublished - Jun 2 1991
Externally publishedYes

ASJC Scopus subject areas

  • Electronic, Optical and Magnetic Materials
  • Ceramics and Composites
  • Condensed Matter Physics
  • Materials Chemistry

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