title: Irreducible finite-size effects in the surface free energy of NaCl crystals from crystal-nucleation data.
abstract: In this Letter we report a simulation study in which we compare the solid-liquid interfacial free energy of NaCl at coexistence, gamma_{LS}, with the value that follows from the height of the homogeneous nucleation barrier. The two estimates differ by more than 100%. Smaller discrepancies are found for gamma_{LS} of hard-sphere and of Lennard-Jones particles. We consider a variety of possible causes for this discrepancy and conclude that it is due to a finite-size effect that cannot be corrected for by any simple thermodynamic procedure. By taking into account the finite-size effects of gamma_{LS} obtained in real nucleation experiments, we obtain quantitative agreement between gamma_{LS} estimated in the simulations and derived from the experiments. Our finding suggests that most published solid-liquid surface free energies derived from nucleation experiments will have to be revised.
authors.affiliation: Department of Chemistry and Applied Biosciences, ETHZ, 6900 Lugano, Switzerland.
authors.forename: T
authors.initials: T
authors.lastname: Zykova-Timan
authors.forename: C
authors.initials: C
authors.lastname: Valeriani
authors.forename: E
authors.initials: E
authors.lastname: Sanz
authors.forename: D
authors.initials: D
authors.lastname: Frenkel
authors.forename: E
authors.initials: E
authors.lastname: Tosatti