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Generalized van der Waals Theory of Interfaces in Simple Fluid Mixtures.

An efficient implementation of the generalized van der Waals theory of fluids is presented for the calculation of surface tension in simple fluid mixtures. While detailed correlation analysis is avoided the dominant binding energy contribution and the negative contribution due to the nonlocal entropy are accounted for in the free energy density functional by simple physical approximations of the type originally introduced by van der Waals. Efficient computation is achieved by the use of a single-parameter optimization of a tanh-shaped profile representing the total density as well as the composition variation across the interface. This simple profile nevertheless incorporates the expected adsorption to the interface of the volatile component. Application is made to argon/krypton mixtures represented by Lennard-Jones potentials and Lorentz-Berthelot combining rules. Surface tension predictions compare well with both experimental observations and computer simulation results which also indicated close agreement in particle density profiles, especially if the Berthelot rule is amended with a binary interaction parameter slightly (3%) less than unity. Copyright 2001 Academic Press.