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Effects of geometrical and energetic nonadditivity on the phase behavior of two-component symmetric mixtures.

Using Monte Carlo simulation methods in the grand-canonical ensemble, we have studied the phase behavior of three-dimensional symmetric binary mixtures of Lennard-Jones particles. We have also elucidated the effects of geometric and energetic nonadditivity on the phase behavior. Phase diagrams for several systems have been evaluated. We have demonstrated that in completely miscible mixtures the geometrical nonadditivity (negative as well as positive) stabilizes a liquid phase leading to a gradual increase of the critical temperature. The mechanism leading to such behavior is different when the system shows negative and positive geometrical nonadditivity. In the case of systems with negative energetic nonadditivity, which may exhibit demixing transition in the liquid phase, their phase behavior is also strongly affected by the geometric non-additivity. The systems with negative geometric nonadditivity have been demonstrated to show reentrant miscibility, while those with positive geometric nonadditivity show enhanced tendency toward mixing at sufficiently high temperatures. We have evaluated phase diagrams for several systems.