Surface Fluctuations Dominate the Slow Glassy Dynamics of Polymer-Grafted Colloid Assemblies

[Image: see text] Colloids grafted with a corona layer of polymers show glassy behavior that covers a wide range of fragilities, with this behavior being tunable through variations in grafting density and grafting chain length. We find that the corona roughness, which is maximized for long chain lengths and sparse grafting, is directly correlated to the concentration-dependence of the system relaxation time (fragility). Relatively rougher colloids result in stronger liquids because their rotational motions become orientationally correlated across the whole system even at low particle loadings leading to an essentially Arrhenius-like concentration-dependence of the relaxation times near the glass transition. The smoother colloids do not show as much orientational correlation except at higher densities leading to fragile behavior. We therefore propose that these materials are an ideal model to study the physical properties of the glass transition.