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Structure formation and aging in different arrested states of Laponite dispersions have been investigated at the macro- and microscale. Covering a wide range of solid content and salt concentrations at different pH glasses, strong and weak gels with prevailing edge-to-face (EF) or face-to-face (FF) layer contacts were formed. Mechanical shear and squeeze flow rheometry were combined with diffusing wave spectroscopy and multiple particle tracking (MPT) microrheology. Strong attractive gels form much more quickly than weak gels, and particularly repulsive glasses. Gels with preferred EF contacts are stronger and are created more quickly than gels with prevailing FF contacts. Strong gels show little aging and exhibit a weak increase of G′ ∼ tα with α = 0.11 ± 0.03, higher α values are found for weak gels, and the strongest aging is observed in glasses. MPT data reveal structural refinement at the submicrometer length scale during aging for gels but not for glasses. Strong structural heterogeneity most pronounced at pH = 8.5 occurs during gel or glass formation, but at longer times, all arrested states appear homogenous at the 0.2 μm length scale. Finally, all arrested states exhibit power law frequency dependence G″ ∼ ω0.75 at high frequencies attributed to internal bending modes of layers.Structure formation and aging in different arrested states of Laponite dispersions have been investigated at the macro- and microscale. Covering a wide range of solid content and salt concentrations at different pH glasses, strong and weak gels with prevailing edge-to-face (EF) or face-to-face (FF) layer contacts were formed. Mechanical shear and squeeze flow rheometry were combined with diffusing wave spectroscopy and multiple particle tracking (MPT) microrheology. Strong attractive gels form much more quickly than weak gels, and particularly repulsive glasses. Gels with preferred EF contacts are stronger and are created more quickly than gels with prevailing FF contacts. Strong gels show little aging and exhibit a weak increase of G′ ∼ tα with α = 0.11 ± 0.03, higher α values are found for weak gels, and the strongest aging is observed in glasses. MPT data reveal structural refinement at the submicrometer length scale during aging for gels but not for glasses. Strong structural heterogeneity most prono...

Macro- and microscale structure formation and aging in different arrested states of Laponite dispersions