Although
recent experimental studies have demonstrated that H2 and
D2 molecules wet the inner surface of supergrowth
carbon nanotubes at low temperatures, characterization of the structural
and dynamical properties in this regime is challenging. This Letter
presents a theoretical study of self-diffusion in pure and binary
H2, D2, and T2 contact monolayer
films formed on the inner surface of a carbon nanotube. Our results
show that monolayer formation and self-diffusion both in pure hydrogen
isotopes and in H2/T2 and H2/D2 isotope mixtures is impacted by nuclear quantum effects,
suggesting potential applications of carbon nanotubes for the separation
of hydrogen isotopes.