Excluded volume effect on polymer dynamics in concentrated solutions

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Abstract
We consider the dynamics of polymers in concentrated solutions under the combined effects of excluded volume interactions and hydrodynamical interactions (including all inter‐ and intrachain effects). Exact dynamical equations are derived which describe the motion of a single chain with screened hydrodynamics in the presence of the instantaneous excluded volume field of all other chains, an exact equation representing the precursor to all reptationlike models. Analogous equations are also obtained for the dynamics of a pair of correlated chains, e.g., ones involved in a temporary entanglement in a concentrated system. For the uncorrelated case of phantom chains, Edwards’s results for the excluded volume effect on equilibrium properties are incorporated into the averaged dynamics to determine the excluded volume effect on the polymer viscosity and the effective bead friction coefficient in concentrated solutions. Experimental viscoelastic data for concentrated solutions and melts are shown to provide a basis for the use of phantom chain models when the polymer chain lengths do not become too large. The effective bead friction coefficient is used in an accompanying paper, along with the dynamical equations derived here, to study quasielastic neutron scattering cross sections from concentrated polymer solutions.

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