SearcharxivSearch

arXiv subjects

Rahul Mangal

Publications and source records attributed to Rahul Mangal.

13 recordsLinked to original sources

Motility and interfacial instability of confined chemically active droplets

Microorganisms navigating through narrow spaces encounter significant hydrodynamic challenges. To overcome these constraints and sustain efficient motion, they employ adaptive strategies, including adaptive oscillatory body deformations. While artificial microdroplets can traverse channels narrower than their diameter, studies of their locomotion have thus far been largely restricted to steady-shape regimes. In this work, we demonstrate a transition from steady shape to dynamic interfacial undulations in 5CB (4'-pentyl-4-cyanobiphenyl) droplets within aqueous trimethylammonium bromide (TTAB) solutions. We show that while droplets in dilute, additive-free solutions maintain a steady shape, the introduction of solutes or higher surfactant concentrations triggers pronounced interfacial undulations. Notably, both steady and undulating droplets exhibit a comparable velocity dependence on the confinement ratio, characterized by an initial deceleration followed by saturation, governed by the competition between hydrodynamic resistance and phoretic flow within the lubrication film. Furthermore, we find that increased surfactant concentration increases the capillary number, resulting in a thicker lubrication layer that facilitates a symmetry-breaking transition. Upon varying confinement, the droplet interface shifts from bilateral undulations to a mode localized on one side, forming a traveling-wave pattern strongly coupled to flow field fluctuations at the droplet's anterior. Linear stability analysis identifies the Yih-Marangoni instability as the underlying mechanism for these oscillations, revealing a previously unrecognized mode of adaptive locomotion in confined active matter.

cond-mat.soft

Clustering Dynamics of SiO2-Pt Active Janus Colloids

Active colloid clustering is central to understanding non-equilibrium self-organization, with implications for programmable active materials and synthetic or biological assemblies. While most prior studies have focused on dimers or small aggregates, the dynamics of larger clusters remain relatively unexplored. Here, we experimentally investigate chemically active, monodisperse SiO2-Pt Janus colloid (JC) clusters as large as n=9 in a dynamic clustering regime, where clusters continuously form, dissolve, and merge as swimmer density increases. We show that clusters move in circular trajectories, and that both their translational and rotational dynamics can be predicted directly from the orientations of constituent JCs. Furthermore, we identify that their formation undergoes a mechanistic transition: while small clusters are mediated by chemical interactions, larger clusters are predominantly formed by steric effects. This transition arises from a mismatch of motilities between incoming JCs and clusters, combined with increased Pt-surface exposure. Our results extend prior dimer-focused studies to larger aggregates and establish a predictive description that bridges individual swimmer behavior with collective dynamics.

cond-mat.soft

Emergence of Order in Chemically Active Droplets: Temporal Dynamics and Collective Behavior

Collective behaviors such as swarming, chemical signaling, and clustering are fundamental to biological microorganisms, enabling hierarchical colony formation, coordinated motion, and enhanced nutrient accessibility crucial for their survival. Over the past few decades, extensive research has been dedicated to unraveling the mechanisms underlying these diverse collective patterns through experimental model systems. Among these, active droplets have emerged as valuable synthetic analogs, effectively replicating key biological attributes and serving as ideal platforms for investigating collective phenomena. This research explores the collective behavior of 4-Cyano-4-pentyl-biphenyl (5CB) oil droplets across varying P\'eclet ($Pe$) numbers. At high $Pe$, droplets exhibit a pusher mode of propulsion and form dynamic chain-like patterns. Decreasing $Pe$ enhances repulsive interactions among droplets, resulting in the inhibition of clustering. In the low $Pe$ regime, their repulsive interactions predominated by chemical field lead to the emergence of an ordered structure. Furthermore, we illustrate how active droplets efficiently navigate within a soft structured environment. These findings contribute to our comprehension of self-organized phenomena in active matter systems and provide insights for designing strategies for controlled locomotion in intricate fluidic environments.

cond-mat.soft

Chemical interactions in active droplets

Interactions among biologically active agents is facilitated by their self-generated chemical and hydrodynamic fields. In order to elucidate the pair-wise interactions between such micro-organisms, we employ active droplets as a model system, capable of self-generating chemical and hydrodynamic fields. We demonstrate that the solute P\'eclet number ($Pe$), characterizing the relative strength of its convective to diffusive transport, plays a crucial role in determining how the chemical and hydrodynamic fields impact their interactions. Our findings reveal that at low $Pe$, the interaction is predominantly governed by chemo-repulsive effects, leading to droplets avoiding physical contact. Conversely, at elevated $Pe$, hydrodynamic interactions become more influential, leading to physical engagement. However, irrespective of $Pe$, the interaction of a droplet with the chemical trail of another droplet is always governed by chemo-repulsive effects. Furthermore, our results establish that the chemo-repulsive deflection/rebounding of droplets is influenced by the droplets' inherent chemical polarity, as determined by its $Pe$, independent of their approach orientation. Our findings offer a methodology for tuning the outcomes of binary interactions among chemically active droplets, laying the groundwork for potential studies on their collective dynamics.

cond-mat.soft

Motility and pair-wise interactions of chemically active droplets in 1-D confinement

Self-propelled droplets serve as ideal model systems to delve deeper into understanding of the motion of biological micro-swimmers by simulating their motility. Biological microorganisms are renowned for showcasing a diverse array of dynamic swimming behaviors when confronted with physical constraints. This study aims to elucidate the impact of physical constraints on swimming characteristics of biological microorganisms. To achieve this, we present observations on the individual and pair-wise behavior of micellar solubilized self-propelled 4-Cyano-4'-pentyl-biphenyl (5CB) oil droplets in a square capillary channel filled with a surfactant trimethyl ammonium bromide (TTAB) aqueous solution. To explore the effect of the underlying Péclet ($Pe$) number of the swimming droplets, the study is also performed in the presence of additives such as high molecular weight polymer Polyethylene oxide (PEO) and molecular solute glycerol. The capillary confinement restricts droplet to predominantly one-dimensional (1D) motion, albeit with noticeable differences in their motion across the three scenarios. Through a characterization of the chemical and hydrodynamic flow fields surrounding the droplets, we illustrate that the modification of the droplets' chemical field due to confinement varies significantly based on the underlying differences in the Péclet number ($Pe$) in these cases. This alteration in the chemical field distribution notably affects the individual droplets' motion. Moreover, these distinct chemical field interactions between the droplets also lead to variations in their pair-wise motion, ranging from behaviors like chasing to scattering.

cond-mat.soft

Pair-Interactions of Self-Propelled SiO2-Pt Janus Colloids: Chemically Mediated Interactions

Driven by the necessity to achieve a thorough comprehension of the bottom-up fabrication process of functional materials, this experimental study investigates the pair-wise interactions or collisions between chemically active SiO2-Pt Janus Colloids. These collisions are categorized based on the Janus colloids orientations before and after they make physical contact. In addition to the hydrodynamic interactions, the Janus colloids are also known to affect each others chemical field, resulting in chemophoretic interactions, which depend on the degree of surface anisotropy in reactivity and solute-surface interaction. These interactions lead to a noticeable decrease in particle speed and changes in orientation that correlate with the contact duration and yield different collision types. Our findings reveal distinct configurations of contact during collisions, whose mechanisms and likelihood is found to be dependent primarily on the chemical interactions. Such estimates of collision and their characterization in dilute suspensions shall have key impact in determining the arrangement and time scales of dynamical structures and assemblies of denser suspensions, and potentially the functional materials of the future.

cond-mat.soft

Mode-Switching of Active Droplets in Macromolecular Solutions

Typical bodily and environmental fluids encountered by biological swimmers consist of dissolved macromolecules such as proteins and polymers, often rendering them non Newtonian. To mimic such scenarios, we investigate the motion of swimming droplets in an ambient medium doped with polymers as macromolecular solutes. Active droplets mimic the essential propulsive characteristics of several biological swimmers and serve as ideal model systems to widen our understanding of their locomotive strategies. Our experiments reveal extreme sensitivity of droplet motion to the presence of macromolecular solutes in the ambient medium. Through in-situ visualization of the self-generated chemical field around the droplet, we report unexpectedly high diffusivity of filled micelles in the presence of high molecular weight polymer solutes or macromolecules. This is attributed to the limitation of Stokes-Einstein relationship in accurately predicting micelle diffusivity due to significant size disparity between micelles and the macromolecular solute. With an increase in polymer concentration, particle image velocimetry reveals a mode-switching, from the conventional pusher mode to a puller mode of propulsion, characterized by a more persistent droplet motion. With a further increase in concentration, a secondary transition from smooth to a jittery mode of propulsion occurs. A robust Peclet number framework is proposed that successfully captures the observed mode-switching of active droplets. Our experiments unveil a novel route to orchestrate complex transitions in active droplet propulsion by doping the ambient medium with suitable choice of macromolecules.

cond-mat.soft

Deforming Active Droplets in Viscoelastic Media

To mimic the motion of biological swimmers in bodily fluids, a novel experimental system of micellar solubilization driven active droplets in a visco-elastic polymeric solution is presented. The visco-elastic nature of the medium, characterized by the Deborah number (De), is tuned by varying the surfactant (fuel) and polymer concentration in the ambient medium. At moderate De, the droplet exhibits a steady deformed shape, markedly different from the spherical shape observed in Newtonian media. A theoretical analysis based on the normal stress balance at the interface is shown to accurately predict the droplet shape. With a further increase in De, time-periodic deformations accompanied by oscillatory transitions in swimming modes are observed. The study unveils the rich complexity in the motion of active droplets in viscoelastic fluids, which has been hitherto unexplored.

cond-mat.soft

Droplet Migration in the Presence of a Reacting Surfactant at Low Péclet Numbers

A surfactant-laden droplet of one fluid dispersed in another immiscible fluid serves as an artificial model system capable of mimicking microbial swimmers. Either an interfacial chemical reaction or the process of solubilization generates gradients in interfacial tension resulting in a Marangoni flow. The resulting fluid flow propels the droplet toward a region of lower interfacial tension. The advective transport of surfactants sustains the active propulsion of these droplets. In these systems, the local interfacial tension is affected by the interfacial reaction kinetics as well as convection and diffusion induced concentration gradients. The migration of such a surfactant-laden viscous droplet undergoing an interfacial reaction, suspended in a background Poiseuille flow is investigated. The focus is specifically on the role of the surface reaction that generates a non-uniform interfacial coverage of the surfactant, which in turn dictates the migration velocity of the droplet in the background flow. Assuming negligible interface deformation and fluid inertia, the Lorentz reciprocal theorem is used to analytically determine the migration velocity of the droplet using regular perturbation expansion in terms of the surface Péclet number. We show that the presence of interfacial reaction affects the magnitude of both stream-wise and cross-stream migration velocity of the droplet in a background Poiseuille flow. We conclude that the stream-wise migration velocity is not of sufficient strength to exhibit positive rheotaxis as observed in recent experimental observations. Additional effects such as the hydrodynamic interactions with the adjacent wall may be essential to capture the same.

physics.flu-dyn

Rheotaxis of Active Droplets

Rheotaxis is a well-known phenomenon among microbial organisms and artificial active colloids, wherein the swimmers respond to an imposed flow. We report the first experimental evidence of upstream rheotaxis by spherical active droplets. It is shown that the presence of a nearby wall and the resulting strong flow-gradient at the droplet level is at the root of this phenomenon. Experiments with optical cells of different heights reveal that rheotaxis is observed only for a finite range of shear rates, independent of the bulk flow-rate. We conjecture that the flow induced distortion of an otherwise isotropic distribution of filled/empty micelles around the droplet propels it against the flow. We also show that nematic droplets exhibit elastic stress-induced oscillations during their rheotactic flight. A promising potential of manipulating the rheotactic behavior to trap as well as shuttle droplets between target locations is demonstrated, paving way to potentially significant advancement in bio-medical applications.

cond-mat.soft

Interaction of Active Janus Particles with Passive Tracers

In this study, we investigated the motion of active SiO2-Pt Janus particles in the 2D bath of smaller silica tracers dispersed in varying areal densities. The effect on the organization of the tracer particles around the active JPs was also explored. Our experiments indicate that the interaction between the tracers and the active JPs mainly depend on the nature of collision marked by the duration of contact. For all the concentration regimes, we have shown that the short time collisions do not have significant impact on the motion of active JPs, however, during moderate/long-time collisions tracer(s) can lead to a significant change in active JPs motion and even cause them to rotate. In the concentrated regime, our experiments reveal the emergence of a novel organizational behavior of the passive tracers on the trailing Pt and the leading SiO2 with a strong dependence on the nature of collision.

cond-mat.soft

Solute Induced Jittery Motion of Self-Propelled Droplets

The intriguing role of the presence of solutes in the activity of a self-propelling droplet is investigated. A system of self-propelling micron sized 4-pentyl-4-biphenylcarbonitrile (5CB) droplets in an aqueous solution of tetradecyltrimethylammonium bromide (TTAB) as surfactant is considered. It is shown that addition of glycerol causes the active 5CB droplet to exhibit a transition from smooth to jittery motion. The motion is found to be independent of the droplet size and the nematic state of 5CB. Analogous experiments with Polyacrylamide (PAAm), Polyvinylpyrrolidone (PVP) and Polyvinyl Alcohol (PVA), as solutes confirm that such a transition cannot merely be explained solely based on the viscosity or Peclet number of the system. We propose that the specific nature of physicochemical interactions between the solute and the droplet interface is at the root of this transition. The experiments show that the time-scales associated with the influx and redistribution of surfactants at the interface are altered in the presence of solutes. Glycerol and PVP significantly enhance the rate of solubilization of the 5CB droplets resulting in a quicker re-distribution of the adsorbed TTAB molecules on the interface, causing the droplet to momentarily stop and then restart in an independent direction. On the other hand, low solubilization rates in the presence of PAAm and PVA lead to smooth trajectories. Our hypothesis is supported by the time evolution of droplet size and interfacial velocity measurements in the presence and absence of solute. Overall, our results provide fundamental insights into the complex interactions emerging due to the presence of solutes.

cond-mat.soft

Self-Propelled Janus Colloids in Shear Flow

To fully harness the potential of artificial active colloids, investigation of their response to various external stimuli including external flow is of great interest. Therefore, in this study, we perform experiments on SiO2-Pt Janus particles suspended in an aqueous medium in a capillary subjected to different shear flow rates. Particles were propelled using varied H2O2 (fuel) concentrations. For a particular propulsion speed, with increasing shear flow, a transition of motion of active Janus particles from the usual random active motion to preferential motion across stream-lines and then finally to migration along the flow, was observed. Our analysis revealed that these transitions are dictated by the torque due to the self-propulsion near wall w.r.t. shear-induced torque. Interestingly, we found that only when these torques are comparable, particles align in a manner such that they migrate significantly across the streamlines.

cond-mat.soft