Adsorption and Electrokinetics at Silica-Electrolyte Interfaces: A Molecular Simulation Study

Experimentally investigating the nanoscale behavior at oxide-electrolyte interfaces has proven to be extremely challenging. Molecular Dynamics (MD) simulations have arisen as a potential computational alternative to gain atomic level insights at these interfaces. But how accurately do these simulations represent the physics and chemistry at the interface? In many situations we do in fact not know. Validation at the interface remains challenging. The force fields used in MD simulations, that describe the inter-particle interactions, are generally optimized for purposes deviating considerably from interfaces. Yet, these same force fields are blindly used to model surface-fluid interactions, yielding wildly varying results of for example ion adsorption. This dissertation tackles the problem of simulating interfaces by critically looking at MD simulations and proposing novel solutions, both for MD simulations in general and specifically targeting their validity and limitations with regards to modeling interfaces…