Rheological signatures of a glass-glass transition in an aging colloidal clay

The occurrence of non-equilibrium transitions between arrested states has recently emerged as an intriguing issue in the field of soft glassy materials. The existence of one such transition has been suggested for aging colloidal clays (Laponite((R)) suspensions) at a weight concentration of 3.0%, although further experimental evidences are necessary to validate this scenario. Here, we test the occurrence of this transition for spontaneously aged (non-rejuvenated) samples by exploiting the rheological tools of dynamical mechanical analysis. On imposing consecutive compression cycles to differently aged clay suspensions, we find that quite an abrupt change of rheological parameters occurs for ages around three days. For Young's and elastic moduli, the change with the waiting time is essentially independent from the deformation rate, whereas other "fluid-like" properties, such as the loss modulus, do clearly display some rate dependence. We also show that the crossover identified by rheology coincides with deviations of the relaxation time (obtained through x-ray photon correlation spectroscopy) from its expected monotonic increase with aging. Thus, our results robustly support the existence of a glass-glass transition in aging colloidal clays, highlighting characteristic features of their viscoelastic behavior.