Individual chemically active drops suspended in a surfactant solution were observed to self-propel spontaneously with straight, helical, or chaotic trajectories. To elucidate how these drops can exhibit such strikingly different dynamics and "decide" what to do, we propose a minimal axisymmetric model of a spherical active drop, and show that simple and linear interface properties can lead to both steady self-propulsion of the droplet as well as chaotic behavior. The model includes two different mobility mechanisms, namely, diffusiophoresis and the Marangoni effect, that convert self-generated gradients of surfactant concentration into the flow at the droplet surface. In turn, surface-driven flow initiates surfactant advection that is the only nonlinear mechanism and, thus, the only source of dynamical complexity in our model. Numerical investigation of the fully-coupled hydrodynamic and advection diffusion problems reveals that strong advection (e.g., large droplet size) may destabilize a steadily self-propelling drop; once destabilized, the droplet spontaneously stops and a symmetric extensile flow emerges. If advection is strengthened even further in comparison with molecular diffusion, the droplet may perform chaotic oscillations. Our results indicate that the thresholds of these instabilities depend heavily on the balance between diffusiophoresis and the Marangoni effect. Using linear stability analysis, we demonstrate that diffusiophoresis promotes the onset of high-order modes of monotonic instability of the motionless drop. We argue that diffusiophoresis has a similar effect on the instabilities of a moving drop.
Experimental observations indicate that chemically active droplets suspended in a surfactantladen fluid can self-propel spontaneously. The onset of this motion is attributed to a symmetrybreaking Marangoni instability resulting from the nonlinear advective coupling of the distribution of surfactant to the hydrodynamic flow generated by Marangoni stresses at the droplet's surface. Here, we use weakly nonlinear analysis to characterize the self-propulsion near the instability threshold and the influence of the droplet's deformability. We report that in vicinity of the threshold, deformability enhances self-propulsion of viscous droplets, but hinders propulsion of drops that are roughly less viscous than the surrounding fluid. Our asymptotics further reveals that droplet deformability may alter the type of bifurcation leading to symmetry breaking: for moderately deformable droplets the onset of self-propulsion is transcritical and a regime of steady self-propulsion is stable; while in the case of highly deformable drops, no steady flows can be found within the asymptotic limit considered in this paper suggesting that the bifurcation is subcritical.
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