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Heat capacity of multilayer methane on graphite: Phase transitions in the first four layers.

We present high-resolution heat-capacity data for methane adsorbed on graphite for nominal coverages of 0.87 to 7 layers, from T = 70 to 120 K. For films thicker than 1.1 layers, we find capillary condensate coexisting with the film. We have performed heat-capacity scans on films formed by both adsorption and desorption. By comparing the locations of the phase transitions in the chemical potential mu vs T plane, we find that there is no significant interaction between the film and the capillary condensate. The heat-capacity signals from the films map out an unexpectedly rich set of phenomena for the second, third, and fourth layers, including a two-dimensional triple point and a liquid-gas coexistence region for each layer. The fourth-layer critical temperature we find is lower than previous values found by vapor-pressure isotherms.