Buoyancy-Driven Chemohydrodynamic Patterns in A + B → Oscillator Two-Layer Stratifications

Abstract

Chemohydrodynamic patterns due to the interplay of buoyancy-driven instabilities and reaction-diffusion patterns are studied experimentally in a vertical quasi-two-dimensional reactor in which two solutions A and B containing separate reactants of the oscillating Belousov-Zhabotinsky system are placed in contact along a horizontal contact line where excitable or oscillating dynamics can develop. Different types of buoyancy-driven instabilities are selectively induced in the reactive zone depending on the initial density jump between the two layers, controlled here by the bromate salt concentration. Starting from a less dense solution above a denser one, two possible differential diffusion instabilities are triggered depending on whether the fast diffusing sulfuric acid is in the upper or lower solution. Specifically, when the solution containing malonic acid and sulfuric acid is stratified above the one containing the slow-diffusing bromate salt, a diffusive layer convection (DLC) instability is observed with localized convective rolls around the interface. In that case, the reaction-diffusion wave patterns remain localized above the initial contact line, scarcely affected by the flow. If, on the contrary, sulfuric acid diffuses upward because it is initially dissolved in the lower layer, then a double-diffusion (DD) convective mode develops. This triggers fingers across the interface that mix the reactants such that oscillatory dynamics and rippled waves develop throughout the whole reactor. If the denser solution is put on top of the other one, then a fast developing Rayleigh-Taylor (RT) instability induces fast mixing of all reactants such that classical reaction-diffusion waves develop later on in the convectively mixed solutions.