Structure, stability and electronic properties of tricycle type graphane

We propose a new allotrope of graphane (named as ‘tricycle') with equivalent 4up/2down UUUDUD hydrogenation in each six‐carbon ring, which can be considered as the combination of previously proposed 3up/3down chair graphane and stirrup graphane. We find that tricycle graphane is more stable than stirrup graphane and its negative Gibbs free energy (–91 meV/atom) is very close to that of the most stable chair one (–103 meV/atom). Investigations on its vibrational property confirm its dynamical stability. Such a new two‐dimensional hydrocarbon may be produced in the process of graphene hydrogenation with a relatively high probability due to its remarkable stability.