This talk will highlight recent developments enabling first principles Monte Carlo (FPMC) simulations for which the potential energy is calculated on-the-fly using Kohn-Sham density functional theory. Applications of FPMC to the prediction of (a) adsorption isotherms for gas molecules in metal-organic frameworks with under-coordinated metal nodes and (b) reaction equilibria in cation-exchanged zeolites. Emphasis will be given to simulation methodologies and microscopic-level origins of the observed thermodynamic behavior.
