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Nanoparticles can greatly enhance the mechanical response of elastomericpolymers essential to a wide range of applications, yet their precise molecularmechanisms of high-strain reinforcement remain largely unresolved. Here weshow, based on molecular dynamics simulations, that high-strain reinforcementemerges from an interplay between granular nanoparticulate compressive behaviorin the normal direction and polymer incompressibility. This feedback loop,which is initiated by a mismatch in the Poisson ratios of nanofiller andpolymer, invokes a contribution from the polymer's bulk modulus to theelongational stress, while the tendency of the polymer to contract in thenormal direction maintains a near-jammed filler state. This effect persistseven once the direct filler elongational contribution becomes dissipative afterthe 'Payne effect' yield. These results indicate that direct particle-particlecontact effects, even in the absence of potential augmenting mechanisms such asglassy polymer bridges, can drive the mechanical reinforcement effects typicalof experimental systems.

Central role of filler-polymer interplay in nonlinear reinforcement of elastomeric nanocomposites