There is broad interest in surface functionalization of 2D materials and its related applications. In this work, we present a novel graphene layer transistor fabricated by introducing fluorinated graphene (fluorographene), one of the thinnest 2D insulator, as the gate dielectric material. For the first time, the dielectric properties of fluorographene, including its dielectric constant, frequency dispersion, breakdown electric field and thermal stability, were comprehensively investigated. We found that fluorographene with extremely thin thickness (5 nm) can sustain high resistance at temperature up to 400°C. The measured breakdown electric field is higher than 10 MV cm−1, which is the heightest value for dielectric materials in this thickness. Moreover, a proof-of-concept methodology, one-step fluorination of 10-layered graphene, is readily to obtain the fluorographene/graphene heterostructures, where the top-gated transistor based on this structure exhibits an average carrier mobility above 760 cm2/Vs, higher than that obtained when SiO2 and GO were used as gate dielectric materials. The demonstrated fluorographene shows excellent dielectric properties with fast and scalable processing, providing a universal applications for the integration of versatile nano-electronic devices.

In this study, the scalable and one-step fabrication of single atomic-layer transistors is demonstrated by the selective fluorination of graphene using a low-damage CF4 plasma treatment, where the generated F-radicals preferentially fluorinated the graphene at low temperature (<200 °C) while defect formation was suppressed by screening out the effect of ion damage. The chemical structure of the C-F bonds is well correlated with their optical and electrical properties in fluorinated graphene, as determined by X-ray photoelectron spectroscopy, Raman spectroscopy, and optical and electrical characterizations. The electrical conductivity of the resultant fluorinated graphene (F-graphene) was demonstrated to be in the range between 1.6 kΩ/sq and 1 MΩ/sq by adjusting the stoichiometric ratio of C/F in the range between 27.4 and 5.6, respectively. Moreover, a unique heterojunction structure of semi-metal/semiconductor/insulator can be directly formed in a single layer of graphene using a one-step fluorination process by introducing a Au thin-film as a buffer layer. With this heterojunction structure, it would be possible to fabricate transistors in a single graphene film via a one-step fluorination process, in which pristine graphene, partial F-graphene, and highly F-graphene serve as the source/drain contacts, the channel, and the channel isolation in a transistor, respectively. The demonstrated graphene transistor exhibits an on-off ratio above 10, which is 3-fold higher than that of devices made from pristine graphene. This efficient transistor fabrication method produces electrical heterojunctions of graphene over a large area and with selective patterning, providing the potential for the integration of electronics down to the single atomic-layer scale.