title: A Polarizable and Transferable PHAST CO2 Potential for Materials Simulation.
abstract: Reliable PHAST (Potentials with High Accuracy Speed and Transferability) intermolecular potential energy functions for CO2 have been developed from first principles for use in heterogeneous systems, including one with explicit polarization. The intermolecular potentials have been expressed in a transferable form and parametrized from nearly exact electronic structure calculations. Models with and without explicit many-body polarization effects, known to be important in simulation of interfacial processes, are constructed. The models have been validated on pressure-density isotherms of bulk CO2 and adsorption in three metal-organic framework (MOF) materials. The present models appear to offer advantages over high quality fluid/liquid state potentials in describing CO2 interactions in interfacial environments where sorbates adopt orientations not commonly explored in bulk fluids. Thus, the nonpolar CO2-PHAST and polarizable CO2-PHAST* potentials are recommended for materials/interfacial simulations.
authors.affiliation: Department of Chemistry, University of South Florida , 4202 East Fowler Avenue, CHE 205, Tampa, Florida 33620-5250, United States.
authors.forename: Ashley L
authors.initials: AL
authors.lastname: Mullen
authors.affiliation: Department of Chemistry, University of South Florida , 4202 East Fowler Avenue, CHE 205, Tampa, Florida 33620-5250, United States.
authors.forename: Tony
authors.initials: T
authors.lastname: Pham
authors.affiliation: Department of Chemistry, University of South Florida , 4202 East Fowler Avenue, CHE 205, Tampa, Florida 33620-5250, United States.
authors.forename: Katherine A
authors.initials: KA
authors.lastname: Forrest
authors.affiliation: Department of Chemistry, University of South Florida , 4202 East Fowler Avenue, CHE 205, Tampa, Florida 33620-5250, United States.
authors.forename: Christian R
authors.initials: CR
authors.lastname: Cioce
authors.affiliation: Department of Chemistry, University of South Florida , 4202 East Fowler Avenue, CHE 205, Tampa, Florida 33620-5250, United States.
authors.forename: Keith
authors.initials: K
authors.lastname: McLaughlin
authors.affiliation: Department of Chemistry, University of South Florida , 4202 East Fowler Avenue, CHE 205, Tampa, Florida 33620-5250, United States.
authors.forename: Brian
authors.initials: B
authors.lastname: Space