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Effect of small additive molecules on the structural relaxation of polymermelts is investigated via molecular dynamics simulations. At a constantexternal pressure and a fixed number concentration of added molecules, thevariation of particle diameter leads to a non-monotonic change of therelaxation dynamics of the polymer melt. For non-entangled chains, this effectis rationalized in terms of an enhanced added-particle-dynamics which competeswith a weaker coupling strength upon decreasing the particle size.Interestingly, cooling simulations reveal a non-monotonic effect on the glasstransition temperature also for entangled chains, where the effect of additiveson polymer dynamics is more intricate. This observation underlines theimportance of monomer-scale packing effects on the glass transition inpolymers. In view of this fact, size-adaptive thermosensitive core-shellcolloids would be a promising candidates route to explore this phenomenonexperimentally.

Non-monotonic effect of additive particle size on the glass transition in polymers