A semiempirical simulation methodology: atomistic and ionic dissociation of silica

Abstract

Modeling defects, surfaces and interfaces of silica is complicated by the presence of charged and uncharged states of the atoms, and the existence of local nonstoichiometric structure. The changes in the local molecular environments associated with defects and surfaces are a consequence of changes in the electronic structure away from the bulk values. The ability to capture the electronic structure changes in simulations is highly desirable to study defects and surfaces. Moreover, the properties and problems of interest also require the use of large scale simulations. Hence, a semiempirical methodology is introduced that contains these desirable properties. The model approach is described and results using the model in the absence of long range interactions are presented. The motivation to ignore Coulombic interactions is driven by the desire to understand the model's ability to describe the bonding interactions and to what degree it captures any of the medium and long range order.