We study aging behavior of an aqueous suspension of Laponite as a function of concentration of Laponite, concentration of salt, time elapsed since preparation of suspension (idle time), and temperature by carrying extensive rheological and conductivity experiments. We observe that temporal evolution of elastic moduli, which describes structural build-up and aging, shifts to low times for experiments carried out for higher concentration of Laponite, higher concentration of salt, greater temperature, and longer idle time while preserving the curvature of evolution in the solid regime (elastic modulus greater than viscous modulus). Consequently appropriate shifting of evolution of elastic modulus in the solid regime leads to aging time-idle time-salt concentration-Laponite concentration-temperature superposition. The existence of such a superposition suggests the generic nature of microstructure buildup irrespective of mentioned variables in the explored range. The behavior of shift factors needed to obtain the superposition indicate that the energy barrier associated with structural buildup decreases with an increase in idle time and temperature and decreases linearly with an increase in concentration of Laponite and that of salt. The conductivity experiments show that ionic conductivity of the suspension increases with increasing Laponite concentration, salt concentration, temperature, and very importantly the idle time. We also analyze the interparticle interactions using DLVO theory that suggests an increase in idle time, temperature, and salt concentration increases the height of the repulsive energy barrier while it decreases the width of the same when particles approach each other in a parallel fashion. However when particles approach each other in a perpendicular fashion, owing to dissimilar charges on edge and face, the energy barrier for the attractive interaction is expected to decrease with an increase in idle time, temperature, and salt concentration. Analysis of rheological and conductivity experiments suggests a strong influence of attractive interactions on the low energy structures in an aqueous suspension of Laponite.
We present an effective time approach to predict long and short time rheological behavior of soft glassy materials from experiments carried out over practical time scales. Effective time approach takes advantage of relaxation time dependence on aging time that allows time-aging time superposition even when aging occurs over the experimental timescales. Interestingly experiments on variety of soft materials demonstrate that the effective time approach successfully predicts superposition for diverse aging regimes ranging from subaging to hyper-aging behaviors. This approach can also be used to predict behavior of any response function in molecular as well as spin glasses.
In this work we study the aging behavior of aqueous suspension of Laponite having 2.8 weight % concentration using rheological tools. At various salt concentration all the samples demonstrate orientational order when observed using crossed polarizers. In rheological experiments we observe inherent irreversibility in the aging dynamics which forces the system not to rejuvenate to the same state in the shear melting experiment carried out at a later date since preparation. The extensive rheological experiments carried out as a function of time elapsed since preparation demonstrate the self similar trend in the aging behavior irrespective of the concentration of salt. We observe that the exploration of the low energy states as a function of aging time is only kinetically affected by the presence of salt. We estimate that the energy barrier to attain the low energy states decreases linearly with increase in the concentration of salt. The observed superposition of all the elapsed time and the salt concentration dependent data suggests that the aging that occurs in low salt concentration systems over a very long period is qualitatively similar to the aging behavior observed in systems with high salt concentration over a shorter period.2
Aqueous suspension of nanoclay Laponite undergoes structural evolution as a function of time, which enhances its elasticity and relaxation time. In this work, we employ an effective time approach to investigate long-term relaxation dynamics by carrying out creep experiments. Typically, we observe that the monotonic evolution of elastic modulus shifts to lower aging times, while maxima in viscous moduli get progressively broader for experiments carried out on a later date after preparation (idle time) of the nanoclay suspension. Application of effective time theory produces a superposition of all the creep curves irrespective of their initial state. The resulting dependence of the relaxation time on aging time shows very strong hyper-aging dynamics at short idle times, which progressively weakens to demonstrate a linear dependence in the limit of very long idle times. Remarkably, this behavior of nanoclay suspensions is akin to that observed for polymeric glasses. Consideration of aging as a first-order process suggests that continued hyper-aging dynamics causes cessation of aging. The dependence of relaxation time on aging time, therefore, must attenuate eventually producing linear or weaker dependence on time in order to approach a progressively low-energy state in the limit of very long times as observed experimentally. We also develop a simple scaling model based on a concept of aging of an energy well, which qualitatively captures various experimental observations very well, leading to profound insight into the hyper-aging dynamics of nanoclay suspensions.
We present stress and critical cracking thickness measurements for drying polymer films.
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