Pulsating dissolution of crystalline matter.

Abstract

Fluid-solid reactions result in material flux from or to the solid surface. The prediction of the flux, its variations, and changes with time are of interest to a wide array of disciplines, ranging from the material and earth sciences to pharmaceutical sciences. Reaction rate maps that are derived from sequences of topography maps illustrate the spatial distribution of reaction rates across the crystal surface. Here, we present highly spatially resolved rate maps that reveal the existence of rhythmic pulses of the material flux from the crystal surface. This observation leads to a change in our understanding of the way crystalline matter dissolves. Rhythmic fluctuations of the reactive surface site density and potentially concomitant oscillations in the fluid saturation imply spatial and temporal variability in surface reaction rates. Knowledge of such variability could aid attempts to upscale microscopic rates and predict reactive transport through changing porous media.