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Monolayer films on graphite, remarkably diverse examples of two-dimensional matter, are now well understood in terms of semiempirical interactions. We explore the phase behavior of helium films on two variants of graphene: graphane (graphene coated with H, denoted GH) and graphene fluoride (GF). The behaviors predicted with quantum Monte Carlo differ qualitatively from those on graphite because of the different surface composition, symmetry, and spacing of the adsorption sites. On both substrates we find that the analog of the standard √3 x √3 R30° commensurate state on graphite is unstable. Results include a superfluid ground state for 4He and a fluid ground state for 3He, neither of which has been found for the monolayer film on any substrate; these two-dimensional fluids are anisotropic because of the symmetry imposed by the honeycomb lattice of adsorption sites. In the case of 4He on GF the anisotropy is as large as if the superfluid were restricted to move in a multiconnected space, along the bonds of a honeycomb lattice. The superfluid transition temperature at the ground-state density of 4He on GF (GH) is of order 0.25 (1.1) K. At higher coverages both an incommensurate triangular solid and a commensurate state at filling factor 2/7 are found. [ABSTRACT FROM AUTHOR]

The adsorption geometry of various gases on top of a C60 monolayer is investigated. The potential energy experienced by an adsorbate atom in the vicinity of a C60 molecule consists of Lennard-Jones interactions integrated over the spherical surface of the molecule. The adsorption potential exhibits strongly attractive sites which lead to a commensurate phase. The next adsorption sites are assumed on the basis of the symmetries of the triangular C60 array. The competition between different adsorption phases is solved by energy minimization. The onset pressure of each phase is computed and compared with experimental data for Kr on top of a C60 monolayer.

A low density film on a flat surface is described by an expansion involving the first four virial coefficients. The first coefficient (alone) yields the Henry's law regime, while the next three terms in the expansion correct for the effects of adsorbate-adsorbate interactions, computed within the two-dimensional approximation (a film confined nearly to a plane). The results permit exploration of the idea of universal adsorption behavior, which is compared with experimental data for a number of systems. The idea works well, in general, justifying a general model of adsorption at low to moderate coverage.

We examine the hydrodynamic phonon spectrum of a monolayer film adsorbed on the wall of a spherical pore. Due to the boundary conditions, the monolayer film exhibits a discrete phonon spectrum. The corresponding density of states per unit frequency is thus a set of delta functions, and the heat capacity exhibits Arrhenius behavior at low temperatures. At high temperatures, the heat capacity approaches the C approximately T2 behavior of a two-dimensional monolayer film. Our results for the spherical surface film are compared to previous calculations for films confined to a cylindrical surface.

We employ a simple model to describe the phase behavior of 4He and Ar in a hypothetical porous material consisting of a regular array of infinitely long, solid, parallel cylinders. We find that high porosity geometries exhibit two transitions: from vapor to film and from film to capillary condensed liquid. At low porosity, the film is replaced by a "necking" configuration, and for a range of intermediate porosity there are three transitions: from vapor to film, from film to necking and from necking to a capillary condensed phase.

Using density functional and Monte Carlo methods, we have studied the properties of Ne adsorbed on a Cs surface, focusing on the region at and near saturated vapor pressure (SVP). In the case of Ne/Rb, the experimental data of Hess, Sabatini, and Chan are consistent with the calculations based on an ab initio fluid-substrate potential, while in the Ne/Cs case there is indication that the potential is approximately 9% too deep. In that case, the calculations yield partial drying behavior consistent with the experimental finding of depressed fluid density near the surface, above SVP. However, we find no evidence of a drying transition, a result consistent with the mean-field calculation of Ebner and Saam.

A study is presented of the effects of gas (especially H2) absorption within the interstitial channels of a bundle of carbon nanotubes. The ground state of the system is determined by minimizing the total energy, which includes the molecules' interaction with the tubes, the intertube interaction, and the molecules' mutual interaction (which is screened by the tubes). The consequences of swelling include a reduced threshold pressure for gas uptake and a 2.7% increase in the tubes' breathing mode frequency.