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Enthalpic interactions at the interface between nanoparticles and matrixpolymers is known to influence various properties of the resultant polymernanocomposites (PNC). For athermal PNCs, consisting of grafted nanoparticlesembedded in chemically identical polymers, the role and extent of the interfacelayer (IL) interactions in determining the properties of the nanocomposites isnot very clear. Here, we demonstrate the influence of the interfacial layerdynamics on the fragility and dynamical heterogeneity (DH) of athermal andglassy PNCs. The IL properties are altered by changing the grafted to matrixpolymer size ratio, f, which in turn changes the extent of matrix chainpenetration into the grafted layer. The fragility of PNCs is found to increasemonotonically with increasing entropic compatibility, characterized byincreasing penetration depth. Contrary to observations in most polymers andglass formers, we observe an anti-correlation between the dependence on ILdynamics of fragility and DH, quantified by the experimentally estimatedKohlrausch-Watts-Williams parameter and the non-Gaussian parameter obtainedfrom simulations.

Interfacial Entropic Interactions Tunes Fragility and Dynamic Heterogeneity of Glassy Athermal Polymer Nanocomposite films