arXiv subjects

Vaibhav Raj Singh Parmar

Publications and source records attributed to Vaibhav Raj Singh Parmar.

9 recordsLinked to original sources

arXiv2026

Elasticity-mediated Morphogenesis in Interfacial Colloidal Assemblies

We study the self-assembly of colloidal microgel particles at a quasi-two-dimensional air-water interface of a drying droplet. Using bright-field microscopy, we demonstrate that increasing particle elasticity drives interfacial organization from repulsion-stabilized crystallization to attraction-dominated gelation, via diverse metastable structures including clusters, voids and anisotropic aggregates. Molecular dynamics simulations using an effective potential that captures the interplay between hydrophobic, capillary, steric and dipolar interactions, reproduce the overall phenomenology of the observed colloidal morphogenesis. Our findings establish particle elasticity as a key parameter governing non-equilibrium structural organization of colloids at an interface.

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arXiv2025

Permeability heterogeneity and bulk linear elasticity of displaced clay suspensions determine interfacial pattern morphologies in Hele-Shaw experiments

When a less viscous Newtonian fluid displaces an aging aqueous clay suspension in a confined space, a rich array of interfacial patterns emerges due to a predominantly viscous instability. In the present work, we controlled the mechanical properties of clay suspensions by incorporating additives and studied the interfacial instabilities that resulted when these suspensions were radially displaced by water in a Hele-Shaw cell. When the elasticity of clay was low, the interfacial dynamics exhibited features of nonlinear viscous fingering in heterogeneous media. By tuning the nature and content of additives that delay clay aging, we uncovered two novel propagation mechanisms: pattern growth \textit{via} skewering and zig-zag finger propagation. These patterns have hitherto never been observed in experiments with colloidal systems. For moderate clay elasticities, we demonstrate here that shear-thinning-induced flow anisotropy leads to the formation of dendrites with dominant side branches. As clay elasticity increases due to the incorporation of salts, the energy required to create fractures becomes smaller than that for system-wide yielding. This scenario is characterized by the emergence of viscoelastic fractures. Our work demonstrates that incorporating additives is an effective strategy to manipulate the onset and growth of interfacial instabilities during the confined displacement of clay by miscible Newtonian fluids.

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arXiv2024

Using optical tweezer electrophoresis to investigate clay nanoplatelet adsorption on Latex microspheres in aqueous media

The adsorption of charged clay nanoplatelets plays an important role in stabilizing emulsions by forming a barrier around the emulsion droplets and preventing coalescence. In this work, the adsorption of charged clay nanoplatelets on a preformed Latex microsphere in an aqueous medium is investigated at high temporal resolution using optical tweezer-based single-colloid electrophoresis. Above a critical clay concentration, charged clay nanoplatelets in an aqueous medium self-assemble gradually to form gel-like networks that become denser with increasing medium salinity. In a previous publication [R. Biswas et. al., Soft Matter, 2023, 19, 24007-2416], some of us had demonstrated that a Latex microsphere, optically trapped in a clay gel medium, is expected to attach to the network strands of the gel. In the present contribution, we show that for different ionic conditions of the suspending medium, the adsorption of clay nanoplatelets increases the effective surface charge on an optically trapped Latex microsphere while also enhancing the drag experienced by the latter. Besides the ubiquitous contribution of non-electrostatic dispersion forces in driving the adsorption process, we demonstrate the presence of an electrostatically-driven adsorption mechanism when the microsphere was trapped in a clay gel. These observations are qualitatively verified via cryogenic field emission scanning electron microscopy and are useful in achieving colloidal stabilisation, for example, during the preparation of clay-armoured Latex particles in Pickering emulsion polymerisation.

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arXiv2024

Manipulating crack formation in air-dried clay suspensions with tunable elasticity

Clay, the major ingredient of natural soils, is often used as a rheological modifier while formulating paints and coatings. When subjected to desiccation, colloidal clay suspensions and clayey soils crack due to the accumulation of drying-induced stresses. Even when desiccation is suppressed, aqueous clay suspensions exhibit physical aging, with their elastic and viscous moduli increasing over time as their microscopic structures evolve due to time-dependent inter-particle screened electrostatic interactions. The rate at which aging progresses is estimated from the rate of evolution of the mechanical moduli and can be controlled by changing clay concentration or by incorporating additives. Since physical aging and evaporation should both contribute to the consolidation of drying clay suspensions, we attempt to manipulate the desiccation process \textit{via} alterations of clay and additive concentrations. For a desiccating sample with an accelerated rate of aging, we observe faster consolidation into a semi-solid state and earlier onset of cracks. We estimate the crack onset time, $t_c$, in direct visualization experiments and the elasticity of the drying sample layer, $E$, using microindentation in an atomic force microscope. We demonstrate that $t_c \propto \sqrt{\frac{G_c}{E}}$, where $G_c$, the fracture energy, is estimated by fitting our experimental data to a linear poroelastic model that incorporates the Griffith's criterion for crack formation. Our work demonstrates that early crack onset is associated with lower sample ductility. The correlation between crack onset in a sample and its mechanical properties as uncovered here is potentially useful in preparing crack-resistant coatings and diverse clay structures.

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arXiv2023

Interfacial instabilities in confined displacements involving non-Newtonian fluids

The growth of interfacial instabilities during fluid displacements can be driven by gradients in pressure, viscosity and surface tension, and by applying external fields. Since displacements of non-Newtonian fluids such as polymer solutions, colloidal and granular slurries are ubiquitous in natural and industrial processes, understanding the growth mechanisms and fully-developed morphologies of interfacial patterns involving non-Newtonian fluids is extremely important. In this perspective, we focus on {displacement experiments} wherein competition{s} between capillary, viscous, elastic and frictional forces drive the onset and growth of interfacial instabilities in confined geometries. We conclude by highlighting several exciting open problems in this research area.

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arXiv2023

Emergence of transient reverse fingers during radial displacement of a shear-thickening fluid

A highly sheared dense aqueous suspension of granular cornstarch particles displays rich nonlinear rheology. We had previously demonstrated the growth and onset of interfacial instabilities when shear-thinning cornstarch suspensions were displaced by a Newtonian fluid, and had suggested methods to maximise displacement efficiency [Palak, R. Sathayanath, S. K. Kalpathy and R. Bandyopadhyay, Colloids Surf. A Physicochem. Eng. Asp., 629 (2021) 127405]. In the present work, we explore the miscible displacement of a dense aqueous cornstarch suspension in its discontinuous shear-thickening regime in a quasi-two-dimensional radial Hele-Shaw cell. We systematically study the growth kinetics of the inner interface between water and the cornstarch suspension, and also of the outer interface between the suspension and air. In addition to the growth of interfacial instabilities at the inner interface, we observe a transient withdrawal of the suspension and the formation of fingering instabilities at the outer interface. We demonstrate that these `reverse fingering' instabilities are extremely sensitive to the injection flow rate of water, the gap of the Hele-Shaw cell and the concentration of the displaced cornstarch suspension, {and emerge irrespective of immiscibility between the fluid pair. We believe that as the cornstarch suspension dilates due to the high shear rate imposed by the displacing fluid, the outer suspension-air interface responds with a restoring force, resulting in the penetration of air into the suspension and the formation of reverse fingers. We note that the growth of reverse fingers significantly reduces the displacement efficiency of the suspension. Finally, we demonstrate a correlation in the growth of inner and outer interfacial patterns by computing the velocity with which stresses propagate in the confined dense suspension. Our findings are useful in understanding the flow of granular materials through constrained geometries and can be extended to study stress propagation in shear-thickening materials due to a sudden imposition of high shear rate, such as in impact behaviour.

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arXiv2023

Correlating microscopic viscoelasticity and structure of an aging colloidal gel using active microrheology and cryogenic scanning electron microscopy

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 develop. Our OT-based oscillatory active microrheology experiments allow us to investigate the mechanical responses of the evolving microstructures in aging aqueous clay suspensions of concentrations ranging from 2.5% w/v to 3.0% w/v and at several aging times between 90 and 150 minutes. We repeat such oscillatory measurements for a range of colloidal probe particle diameters and investigate the effect of probe size on the microrheology of the aging suspensions. Using cryogenic field emission scanning electron microscopy (cryo-FESEM), we examine the average pore areas of the Laponite suspension microstructures for various sample concentrations and aging times. By combining our OT and cryo-FESEM data, we report here for the first time to the best of our knowledge, an inverse correlation between the crossover modulus and the average pore diameter of the aging suspension microstructures for the different suspension concentrations and probe particle sizes studied here.

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arXiv2022

Growth kinetics of interfacial patterns formed by the radial displacement of an aging viscoelastic suspension

When a soft glassy colloidal suspension is displaced by a Newtonian fluid in a radial Hele-Shaw geometry, the pattern morphology that develops at the interface is determined by the complex rheology of the former. We had reported in an earlier work [Palak, V. R. S. Parmar, D. Saha and R. Bandyopadhyay, JCIS Open, 6 (2022) 100047] that a range of interfacial patterns can be formed by controlling the elasticity of the displaced suspension, the flow rate of the displacing fluid and the interfacial tension of the fluid pair. Interestingly, all the different morphological features can be distinguished in terms of their areal ratios, defined as the ratio of the areas occupied by the fully-developed pattern and the smallest circle enclosing it. In a significant advance to this earlier work, we show here that a systematic study of spatio-temporal pattern growth can reveal important information about pattern selection mechanisms. We analyse the time-evolution of the patterns to reveal interesting correlations between their growth mechanisms and fully-developed morphologies. We believe that such systematic identification of the unique temporal features characterising pattern growth at the interface between an aging viscoelastic clay suspension and a Newtonian fluid can be useful in predicting and suppressing the onset and evolution of interfacial instabilities in the displacement of mud and cement slurries.

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arXiv2022

Pattern selection in radial displacements of a confined aging viscoelastic fluid

Intricate fluid displacement patterns, arising from the unstable growth of interfacial perturbations, can be driven by fluid viscoelasticity and surface tension. A soft glassy suspension ages, $i.e.$ its mechanical moduli evolve with time, due to the spontaneous formation of suspension microstructures. The shear and time-dependent rheology of an aging suspension can be exploited to generate a wide variety of interfacial patterns during its displacement by a Newtonian fluid. Using video imaging, we report a rich array of interfacial pattern morphologies: dense viscous, dendritic, viscoelastic fracture, flower-shaped, jagged and stable, during the miscible and immiscible displacements of an aging colloidal clay suspension by Newtonian fluids injected into a radial quasi-two-dimensional geometry at different flow rates. We propose a new parameter, the areal ratio, which we define as the fully-developed pattern area normalized by the area of the smallest circle enclosing it. We show that the natural logarithms of the areal ratios uniquely identify the distinct pattern morphologies, such that each pattern can be segregated in a three-dimensional phase diagram spanned by the suspension aging time, the displacing fluid flow rate, and interfacial tension. Besides being of fundamental interest, our results are useful in predicting and controlling the growth of interfaces during fluid displacements.

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