title: Entropic Description of Gas Hydrate Ice-Liquid Equilibrium via Enhanced Sampling of Coexisting Phases.
abstract: Metastable β ice holds small guest molecules in stable gas hydrates, so its solid-liquid equilibrium is of interest. However, aqueous crystal-liquid transitions are very difficult to simulate. A new molecular dynamics algorithm generates trajectories in a generalized NPT ensemble and equilibrates states of coexisting phases with a selectable enthalpy. With replicas spanning the range between β ice and liquid water, we find the statistical temperature from the enthalpy histograms and characterize the transition by the entropy, introducing a general computational procedure for first-order transitions.
authors.affiliation: Department of Chemistry, Boston University, Boston, Massachusetts 02215-2521, USA.
authors.forename: Edyta
authors.initials: E
authors.lastname: Małolepsza
authors.affiliation: Broad Institute of MIT and Harvard, Cambridge, Massachusetts 02142, USA.
authors.forename: Jaegil
authors.initials: J
authors.lastname: Kim
authors.affiliation: Department of Chemistry, Boston University, Boston, Massachusetts 02215-2521, USA.
authors.forename: Tom
authors.initials: T
authors.lastname: Keyes