In this paper we study deformation, failure and breakage of visco-elastic thin films of aging laponite suspension under tensile deformation field. Aqueous suspension of laponite is known to undergo waiting time dependent evolution of its micro-structure, also known as aging, which is accompanied by an increase in the elastic modulus and relaxation time. In the velocity controlled tensile deformation experiments, we observed that the dependence of force and dissipated energy on velocity and initial thickness of the film is intermediate to a Newtonian fluid and a yield stress fluid. For a fixed waiting time, strain at break and dissipated energy increased with velocity, but decreased with initial thickness. With increase in age, strain at break and dissipated energy showed a decrease suggesting enhanced brittle behavior with increase in waiting time, which may be caused by restricted relaxation modes due to aging. In a force controlled mode, decrease in strain at failure at higher age also suggested enhanced brittleness with increase in waiting time. Remarkably, the constant force tensile deformation data up to the point of failure showed experimental time- aging time superposition that gave an independent estimation of relaxation time and elastic modulus dependence on age.
We study aging behavior of 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 modulus, which describes structural buildup and aging, shifts to low times for experiments carried out for higher concentration of Laponite, higher concentration of salt, greater temperature and on higher idle time while preserving the curvature of evolution in the solid regime. Consequently…
We have studied the effect of temperature on aging dynamics of laponite suspensions by carrying out the rheological oscillatory and creep experiments. We observed that at higher temperatures the mechanism responsible for aging became faster thereby shifting the evolution of elastic modulus to lower ages. Significantly, in the creep experiments, all the aging time and the temperature dependent strain data superposed to form a master curve. Possibility of such superposition suggests that the rheological behavior depends on the temperature and the aging time only through the relaxation processes …
The phenomenon of aging in soft matter systems is an intriguing and interesting. In his study we investigate the microstructure and aging dynamics of fluorescent nanoclay gels formed from the mixture of small (~25) and large (~250) aspect ratio nanodiscs using various experimental techniques. We examine how the presence of one kind of clay in other clay of different nature affect the aging dynamics, microstructure and the final resulting phase. Viscosity of the dispersions grows as a power-law with waiting time of the system and the dispersions initially show Maxwellian behaviour but deviated …
Aqueous suspensions of Laponite with discotic particles are well-studied and find a wide range of applications in industry. A new direction of their implementation is polymer composites that can exhibit improved physical properties.We have studied the aging of aqueous suspensions of Laponite and sodium polystyrene sulfonate (PSS-Na) and both their microscopic (small-angle X-ray scattering, SAXS) and macroscopic (small amplitude oscillatory shear (SAOS) rheometry) properties. The concentration of Laponite, $C_L$, was fixed at 2.5% wt and concentration of PSS-Na, $C_p$, was varied within 0-0.5% …
Glasses behave as solids due to their long relaxation time; however the origin of this slow response remains a puzzle. Growing dynamic length scales due to cooperative motion of particles are believed to be central to the understanding of both the slow dynamics and the emergence of rigidity. Here, we provide experimental evidence of a growing dynamical heterogeneity length scale that increases with increasing waiting time in an aging colloidal glass of Laponite. The signature of heterogeneity in the dynamics follows from dynamic light scattering measurements in which we study both the rotation…
This work discusses the sedimentation stability and aging of aqueous suspension of Laponite in the presence of cetyltrimethylammonium bromide (CTAB). The concentration of Laponite was fixed at the constant level $C_l=2$ %wt, which corresponds to the threshold between equilibrium gel IG$_1$ and repulsive gel IG$_2$ phases. The concentration of CTAB $C_s$ was within 0-0.3 %wt. In the presence of CTAB the Laponite aqueous suspensions were unstable against sedimentation and they separated out into upper and bottom layers (U- and B-layers, respectively). The dynamic light scattering technique revea…
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 simil…
Hypothesis: Aging in colloidal suspensions manifests as a reduction in kinetic freedom of the colloids. In aqueous suspensions of charged colloids, the role of inter-particle electrostatics interactions on the aging dynamics is well debated. Despite water being the dispersion medium, the influence of water structure on the physicochemical properties of aging colloids has never been considered before. Laponite, a model hectorite clay, could be used to evaluate the relative contributions of medium structure and electrostatics in determining the physicochemical properties of aging colloidal suspe…
Synthetic Laponite-clay particles with platelet-like shape display strong aging when dispersed in aqueous solutions, preventing latter from reaching their natural liquid-crystalline equilibrium state. Here we introduce a facile method that successfully prevents this aging behaviour and enables accessing the systems' liquid-crystal and crystalline phases. We graft the comb-like polymer, poly(L-lysine)-g-poly(ethylene glycol) (PLL-PEG), onto the clay surfaces from solution, thereby screening the negative surface charges and thus ensuring steric stabilisation. We show zeta-sizer and rheology meas…
Optical tweezers (OTs) can detect pico-Newton range forces operating on a colloidal particle trapped in a medium and have been successfully utilized to investigate complex systems with internal structures. Laponite clay particles in an aqueous medium self-assemble to form microscopic networks over time as electrostatic interactions between the particles gradually evolve in a physical aging process. We investigate the forced movements of an optically trapped micron-sized colloidal probe particle, suspended in an aging Laponite suspension, as the underlying Laponite microstructures gradually dev…
The primary and secondary relaxation timescales of aging colloidal suspensions of Laponite are estimated from intensity autocorrelation functions obtained in dynamic light scattering (DLS) experiments. The dynamical slowing down of these relaxation processes are compared with observations in fragile supercooled liquids by establishing a one-to-one mapping between the waiting time since filtration of a Laponite suspension and the inverse of the temperature of a supercooled liquid that is rapidly quenched towards its glass transition temperature. New timescales, such as the Vogel time and the Ka…
An aqueous suspension of the synthetic clay Laponite undergoes a transition from a liquid-like ergodic state to a glass-like nonergodic arrested state. In an observation that closely resembles the dynamical slowdown observed in supercooled liquids, the phenomenon of kinetic arrest in Laponite suspensions is accompanied by a growth in the $α$-relaxation time with increasing sample aging time, $t_{w}$. The ubiquitous dynamic slowdown and fragile behavior observed in glass forming liquids approaching the glass transition is typically ascribed to the growth in the size of distinct dynamical hetero…
We have studied the tensile deformation behaviour of thin films of aging aqueous suspension of Laponite, a model soft glassy material, when subjected to a creep flow field generated by a constant engineering normal stress. Aqueous suspension of Laponite demonstrates aging behaviour wherein it undergoes time dependent enhancement of its elastic modulus as well as its characteristic relaxation time. However, under application of the normal stress, the rate of aging decreases and in the limit of high stress, the aging stops with the suspension now undergoing a plastic deformation. Overall, it is …
Colloidal suspensions that are out of thermodynamic equilibrium undergo physical aging wherein their structure evolves to lower the free energy. In aqueous suspension of Laponite, physical aging accompanies increases of elastic and viscous moduli as a function of time. In this work we study temporal evolution of elastic and viscous moduli at different frequencies and observe that freshly prepared aqueous suspension of Laponite demonstrates identical rheological behavior reported for the crosslinking polymeric materials undergoing chemical gelation. Consequently at a certain time tanδ is observ…
The settling dynamics of falling spheres inside a Laponite suspension is studied. Laponite is a colloidal synthetic clay that shows physical aging in aqueous suspension due to the spontaneous evolution of inter-particle electrostatic interactions. In our experiments, millimeter-sized steel balls are dropped in aqueous Laponite suspensions of different ages (i.e., time elapsed since sample preparation). The motion of the falling balls are captured using a high-speed camera and the velocities of their centroids are estimated from the images. Interestingly, we observe that balls of larger diamete…
In this work we investigate creep flow of aqueous suspension of Laponite, a model soft glassy material, at different aging times and stresses. We observe that this system shows time - aging time - stress superposition over a range of aging times and stresses when real time scale is transformed into effective time scale. Existence of superposition in an effective time domain facilitates prediction of long and very short time rheological behavior. Analysis of the observed behavior from effective time approach suggests that superposition is possible only when the shape of a relaxation time spectr…
Aqueous colloidal Laponite clay suspensions transform spontaneously to a soft solid-like arrested state as its aging or waiting time increases. This article reports the rapid transformation of aqueous Laponite suspensions into soft solids due to the application of a DC electric field. A substantial increase in the speed of solidification at higher electric field strengths is also observed. The electric field is applied across two parallel brass plates immersed in the Laponite suspension. The subsequent solidification that takes place on the surface of the positive electrode is attributed to th…
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 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 modulus gets progressively broader for experiments carried out on a later date since preparation (idle time) of nanoclay suspension. Application of effective time theory produces superposition of all the cre…
We study the rotational diffusion of aging Laponite suspensions for a wide range of concentrations using depolarized dynamic light scattering. The measured orientational correlation functions undergo an ergodic to non-ergodic transition that is characterized by a concentration-dependent ergodicity-breaking time. We find that the relaxation times associated with rotational degree of freedom as a function of waiting time, when scaled with their ergodicity-breaking time, collapse on two distinct master curves. These master curves are similar to those previously found for the translational dynamic…
Dynamic Light Scattering (DLS) measurements were performed on colloidal suspensions of Laponite\textsuperscript{\textregistered} at different concentrations in the range $C_\text{w}= (1.5÷3.0)$%. The slowing down of the dynamics induced by aging was monitored by following the temporal evolution of autocorrelation functions at different concentrations towards the gel and glass transition. Exploiting analogies with supercooled liquids approaching their glass transitions, an Angell plot for the structural relaxation times was drawn. Finally, the fragility of Laponite\textsuperscript{\textregister…
We explore the link between soft vibrational modes and local relaxation events in polymer glasses during physical aging, active deformation at constant strain rate, and subsequent recovery. A softness field is constructed out of the superposition of the amplitudes of the lowest energy normal modes, and found to predict up to 70% of the rearrangements. Overlap between softness and rearrangements increases logarithmically during aging and recovery phases as energy barriers rise due to physical aging, while yielding rapidly rejuvenates the overlap to that of a freshly prepared glass. In the strai…
