S(t)imulating collaboration with Dave Wesolowski: From alpha (rutile) to zeta (potential)

This talk summarizes 15 years of collaboration with Dave Wesolowski on solid​/liq. interfaces, from implementing the Bandura & Kubicki ab initio force field and first mol. dynamics simulations of (110) rutile (α-​TiO2) to recent non-​equil. simulations elucidating the mol. origin of the zeta potential. Along this journey, we have gradually explored more complex properties of the solid-​liq. interface and developed the methodol. to study the distance-​dependent properties of the inhomogeneous interfacial region. Particularly, we have investigated the adsorption of water and ions on neutral and charged surfaces, characterized the local viscosity, diffusivity and dielec. properties of water mols. between surface slabs and described effect of temp. and pH on the dynamics of ions. All these studies lead to deeper understanding of the mol. structure of the Elec. Double Layer, often shattering the simple theor. views (esp. when the mol. structure of water is ignored)​, while being in good agreement with expts. including surface titrns., X-​ray scattering, and electrokinetic measurements. Some issues raised by Dave Wesolowski, which have not been thoroughly investigated so far, will also be discussed.