The aim of this thesis is twofold with both elements related to industrially relevant crystal systems and processes. The first element utilized a combined scanning electrochemical cell microscope (SECCM) and atomic force microscopy (AFM) method to study the dissolution of enamel surfaces with controlled proton flux to the surface. This was then extended to investigate the effect of both known surface treatments, fluoride and zinc ions, but also a novel treatment of calcium silicate and its methods of action. The second element investigated the use of a nanopipette to investigate the early nucleation and initial growth of calcium carbonate crystals.

For the dissolution of enamel, an SECCM probe to selectively etch a surface for a defined period of time with a high spatial resolution was used. The extent of the etching in the resultant pits was then monitored through AFM to measure the volume of material removed along with other pit dimensions. The method allowed for multiple independent measurements on a single sample, which could be selectively treated to eliminate comparability issues associated with measurements on multiple samples. The system could be modelled via finite element method (FEM) to calculate an intrinsic rate of reaction for the proton induced dissolution of enamel. A proton induced rate constant of dissolution of