Modelling excess surface energy in dry and wetted calcite systems

We have combined the calcite force field of Hwang et al. (J. Phys. Chem. B 105:4,122–4,127, 2001) with the F3C water model and a hybrid Lennard-Jones/van der Waals 3-site potential for CO₂ to investigate the (10`1]4){\left({10\overline14}\right)} and ( 10`1]0){\left( {10\overline10}\right)} cleaving surfaces of calcite under dry and wetted conditions. The wetting fluid included both pure water and water–carbon dioxide mixture. Excess surface energies and structural features of the calcite–fluid interface were analyzed, with the simulation results for the relaxed surfaces confirming the experimentally observed morphology and supporting our conclusion that the relative stability order of calcite cleaving surfaces under investigation will remain unchanged in the presence of water–carbon dioxide mixture as well.