Contact and macroscopic ageing in colloidal suspensions

The progressive stiffening of the solid-solid contacts that freeze dense colloidal suspensions are shown to cause the macroscopic ageing of such materials. The ageing behaviour of dense suspensions or pastes at rest is almost exclusively attributed to structural dynamics. Here, we identify another ageing process, contact-controlled ageing, consisting of the progressive stiffening of solid-solid contacts of an arrested colloidal suspension. By combining rheometry, confocal microscopy and particle-scale mechanical tests using laser tweezers, we demonstrate that this process governs the shear-modulus ageing of dense aqueous silica and polymer latex suspensions at moderate ionic strengths. We further show that contact-controlled ageing becomes relevant as soon as Coulombic interactions are sufficiently screened out that the formation of solid-solid contacts is not limited by activation barriers. Given that this condition only requires moderate ion concentrations, contact-controlled ageing should be generic in a wide class of materials, such as cements, soils or three-dimensional inks, thus questioning our understanding of ageing dynamics in these systems.