This thesis is composed of two parts. The first is a study of evolutionary strategies for parametrization of empirical potentials, and their application in development of a charge-transfer potential for silica. An evolutionary strategy was meta-optimized for use in empirical potential parametrization, and a new charge-transfer empirical model was developed for use with isobaric-isothermal ensemble molecular dynamics simulations. The second is a study of thermodynamics and self-assembly in a particular class of athermal two-dimensional lattice models. The effects of shape on self-assembly and thermodynamics for polyominoes and tetrominoes were examined. Many interesting results were observed, including complex clustering, non-ideal mixing, and phase transitions. In both parts, computational efficiency and performance were important goals, and this was reflected in method and program development
