<p><strong>Abstract.</strong> Mineral aerosol particles can act as ice nucleators, and many insights have been obtained on water freezing as a function of mineral surface properties such as the charge or morphology. Previous studies have mainly focused on pristine samples, despite the fact that under natural atmospheric conditions, aerosol particles age. For example, an aerosol-containing cloud droplet can go through different freeze-melt cycles, so that not only the aerosol surface structure may change, but also the ionic strength and pH of the cloud droplet. The potential variation of the surface properties of an ice nucleating particle during its residence in the atmosphere has been largely overlooked. Here, we use an environmental cell in conjunction with nonlinear spectroscopy (second-harmonic generation) to study the effect of freeze-melt processes on aqueous chemistry at silica surface at low pH. We found that the successive freeze-melt cycles disrupt the dissolution equilibrium, substantially changing the surface properties, giving rise to marked variations in the interfacial water structure and the ice nucleation ability of the surface. The degree-of-order of water molecules, next to the surface at a specific temperature, decreases and then increases again with sample aging. The water ordering&#8211;cooling dependence and ice nucleation ability improve continuously.</p>