In situ study of hydrogenation of graphene and new phases of localization between metal-insulator transitions.

Monolayer graphene synthesized by chemical vapor deposition was subjected to controlled and sequential hydrogenation using RF plasma while monitoring its electrical properties in situ. Low-temperature transport properties, namely, electrical resistance (R), thermopower (S), Hall mobility (μ), and magnetoresistance (MR), were measured for each sample and correlated with ex situ Raman scattering and X-ray photoemission (XPS) characteristics. For weak hydrogenation, the transport is seen to be governed by electron diffusion, and low-temperature transport properties show metallic behavior (conductance G remains nonzero as T → 0). For strong hydrogenation, the transport is found to be describable by variable range hopping (VRH) and the low T conductance shows insulating behavior (G → 0 as T → 0). Weak localization (WL) behavior is seen with a negative MR for weakly hydrogenated graphene, and these WL effects are seen to diminish as the hydrogenation progresses. A clear transition to strong localization (SL) is evident with the emergence of pronounced negative MR for strongly hydrogenated graphene.