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The detailed nature of spatially heterogeneous dynamics of glycerol-silicananocomposites is unraveled by combining dielectric spectroscopy with atomisticsimulation and statistical mechanical theory. Analysis of the spatial mobilitygradient shows no 'glassy' layer, but the alpha relaxation time near thenanoparticle grows with cooling faster than the alpha relaxation time in thebulk, and is ~ 20 times longer at low temperatures. The interfacial layerthickness increases from ~ 1.8 nm at higher temperatures to ~ 3.5 nm uponcooling to near Tg. A real space microscopic description of the mobilitygradient is constructed by synergistically combining high temperature atomisticsimulation with theory. Our analysis suggests that the interfacial slowing downarises mainly due to an increase of the local cage scale barrier for activatedhopping induced by enhanced packing and densification near the nanoparticlesurface. The theory is employed to predict how local surface densification canbe manipulated to control layer dynamics and shear rigidity over a widetemperature range.

Revealing spatially heterogeneous relaxation in a model nanocomposite