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The structure of silica-latex nanocomposites of three matrix chain masses(20, 50, and 160 kg/mol of poly(ethyl methacrylate)) are studied using aSAXS/TEM approach, coupled via Monte Carlo simulations of scattering of fullypolydisperse silica nanoparticle aggregates. At low silica concentrations (1vol. %), the impact of the matrix chain mass on the structure is quantified interms of the aggregation number distribution function, highest mass leading toindividual dispersion, whereas the lower masses favor the formation of smallaggregates. Both simulations for SAXS and TEM give compatible aggregatecompacities around 10 vol. %, indicating that the construction algorithm foraggregates is realistic. Our results on structure are rationalized in terms ofthe critical collision time between nanoparticles due to diffusion in viscousmatrices. At higher concentrations, aggregates overlap and form a percolatednetwork, with a smaller and lighter mesh in the presence of high mass polymers.The linear rheology is investigated with oscillatory shear experiments. Itshows a feature related to the silica structure at low frequencies, theamplitude of which can be described by two power laws separated by thepercolation threshold of aggregates.

Tuning Structure and Rheology of Silica-Latex Nanocomposites with the Molecular Weight of Matrix Chains: A Coupled SAXS-TEM-Simulation Approach