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Experiments and computer simulations demonstrate that water spontaneouslyfills the hydrophobic cavity of a carbon nanotube. To gain a quantitativethermody- namic understanding of this phenomenon, we use the recently developedTwo Phase Thermodynamics (2PT) method to compute translational and rotationalentropies of confined water molecules inside single-walled carbon nanotubes andshow that the increase in energy of a water molecule inside the nanotube iscompensated by the gain in its rotational entropy. The confined water is inequilibrium with the bulk wa- ter and the Helmholtz free energy per watermolecule of confined water is the same as that in the bulk within the accuracyof the simulation results. A comparison of translational and rotational spectraof water molecules confined in carbon nanotubes with that of bulk water showssignificant shifts in the positions of the spectral peaks that are directlyrelated to the tube radius.

Thermodynamics of Water Entry in Hydrophobic Channels of Carbon Nanotubes