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ON THE FREE-VOLUME MODEL OF THE LIQUID-GLASS TRANSITION.

D. Turnbull, M. H. Cohen
Published 1970 · Chemistry

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We have improved the free‐volume model for molecular transport in dense fluids, as developed in earlier papers, by taking account of the variable magnitude of the diffusive displacement. The development is carried through in a way which may display more clearly the relation between the free‐volume model and the Enskog theory. Implicit in the free‐volume development is the association, on the average, of a correlation factor f(a) with each magnitude, a, of the displacement. It is assumed that f(a) is a step function which is zero, because of the predominance of back scattering, for a   a.* This corresponds to dividing the displacements sharply into two categories, one “gaslike” and the other “solidlike.” Molecular dynamics computations have shown that the self‐diffusion coefficient in the hard‐sphere fluid at the highest densities is falling precipitously, with increasing density, away from the Enskog values. It appears that this density trend, which was attributed to back scattering, ...
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