Following the long-term evolution of sp³-type defects in tritiated graphene using Raman spectroscopy

We report on the evolution of tritium-induced sp³-defects in monolayer graphene on a Si/SiO₂ substrate, by comparing large-area Raman maps of the same two samples, acquired just after fabrication and twice thereafter, about 9-12 months apart. In-between measurements the samples were kept under standard laboratory conditions. Using a conservative classification of sp³-type spectra, based on the D/D' peak intensity ratio, we observed almost complete depletion of sp³-type defects over the investigation period of about two years. This by far exceeds the ∼5.5% annual reduction expected from tritium decay alone (≥3× larger). This change in the defect composition is accompanied by a recovery of the 2D-band of graphene and an overall decrease in defect-density, as determined via the D/G intensity ratio. Hydrogenated graphene is reported to be reasonably stable over several months, when kept under vacuum, but suffers substantial hydrogen loss under laboratory air conditions. While the results shown here for tritiated graphene exhibit similarities with hydrogenated graphene, however, some distinct differences are observed.