Using grand-canonical molecular dynamics simulations and free energy calculations of spherical molecular confined films, we investigate the internal energy and entropic origins of density layering and solvation force oscillations. We show that these properties, as well as diffusion and rheological characteristics of such films, depend on interfacial commensurability, with commensurate films exhibiting abrupt solidification for relatively thick, 5 or 6 layer, films.

• Received 18 April 1997

DOI:https://doi.org/10.1103/PhysRevLett.79.705