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Cluster Morphology-Polymer Dynamics Correlations in Sulfonated Polystyrene Melts: Computational Study.

Reaching exceptionally long times up to 500 ns in equilibrium and nonequilibrium molecular dynamics simulations studies, we have attained a fundamental molecular understanding of the correlation of ionomer clusters structure and multiscale dynamics, providing new insight into one critical, long-standing challenge in ionic polymer physics. The cluster structure in melts of sulfonated polystyrene with Na^{+} and Mg^{2+} counterions are resolved and correlated with the dynamics on multiple length and time scales extracted from measurements of the dynamic structure factor and shear rheology. We find that as the morphology of the ionic clusters changes from ladderlike for Na^{+} to disordered structures for Mg^{2+}, the dynamic structure factor is affected on the length scale corresponding to the ionic clusters. Rheology studies show that the viscosity for Mg^{2+} melts is higher than for Na^{+} ones for all shear rates, which is well correlated with the larger ionic clusters' size for the Mg^{2+} melts.