Marangoni- vs. buoyancy-driven flows: competition for spatio-temporal oscillations in A + B → C systems

Abstract

The emergence of self-organized behaviors such as spatio-temporal oscillations is well-known for complex reactions involving nonlinear chemical or thermal feedback. Recently, it was shown that local oscillations of the chemical species concentration can be induced under isothermal batch conditions for simple bimolecular A + B → C reactions, provided they are actively coupled with hydrodynamics. When two reactants A and B, initially separated in space, react upon diffusive contact, damped spatio-temporal oscillations could develop when the surface tension increases sufficiently in the reaction zone. Additionally, if the density decreases, the coupling of both surface tension- and buoyancy-driven contributions to the flow can further sustain this oscillatory instability. Here, we investigate the opposite case of a reaction inducing a localized decrease in surface tension and an increase in density in the reacting zones. In this case, the competition arising from the two antagonistic flows is needed to create oscillatory dynamics, i.e., no oscillations are observed for pure chemically driven Marangoni flows. We study numerically these scenarios in a 2-dimensional system and show how they are controlled by the following key parameters: (i) ΔM and ΔR governing the surface tension and density variation during the reaction, respectively, (ii) the layer thickness of the system, and (iii) its lateral length. This work is a further step toward inducing and controlling chemical oscillations in simple reactions.