Tuning the charge carrier density of two-dimensional (2D) materials by incorporating dopants into the crystal lattice is a challenging task. An attractive alternative is the surface transfer doping by adsorption of molecules on 2D crystals, which can lead to ordered molecular arrays. However, such systems, demonstrated in ultra-high vacuum conditions (UHV), are often unstable in ambient conditions. Here we show that air-stable doping of epitaxial graphene on SiC—achieved by spin-coating deposition of 2,3,5,6-tetrafluoro-tetracyano-quino-dimethane (F4TCNQ) incorporated in poly(methyl-methacrylate)—proceeds via the spontaneous accumulation of dopants at the graphene-polymer interface and by the formation of a charge-transfer complex that yields low-disorder, charge-neutral, large-area graphene with carrier mobilities ~70 000 cm² V⁻¹ s⁻¹ at cryogenic temperatures. The assembly of dopants on 2D materials assisted by a polymer matrix, demonstrated by spin-coating wafer-scale substrates in ambient conditions, opens up a scalable technological route toward expanding the functionality of 2D materials.

This study investigated the transport properties of single-layer reduced graphene oxides (rGOs). The rGOs were prepared by the bubble deposition method followed by thermal reduction. The crossover of the transport mechanism from Efros-Shklovskii (ES) variable range hopping (VRH) between the localized states to Mott-VRH was observed near 70 K using the temperature-dependent conductance. The ES-VRH conduction below 70 K is apparent in the electric field dependence of the field-driven hopping transport in the high-electric field regime. We also figure out that the thermoelectric power is consistent with the 2D Mott VRH above 70 K. We argue that the VRH conduction results from the topological disorders of rGO as confirmed by Raman spectroscopy. This infers that the average distance between defects is approximately 2.0 nm.

One of the aspirations of quantum metrology is to deliver primary standards directly to end-users thereby significantly shortening the traceability chains and enabling more accurate products. Epitaxial graphene grown on silicon carbide (epigraphene) is known to be a viable candidate for a primary realisation of a quantum Hall resistance standard, surpassing conventional semiconductor two-dimensional electron gases, such as those based on GaAs, in terms of performance at higher temperatures and lower magnetic fields. The bottleneck in the realisation of a turn-key quantum resistance standard requiring minimum user intervention has so far been the need to fine-tune the carrier density in this material to fit the constraints imposed by a simple cryo-magnetic system. Previously demonstrated methods, such as via photo-chemistry or corona discharge, require application prior to every cool-down as well as specialist knowledge and equipment. To this end we perform metrological evaluation of epigraphene with carrier density tuned by a recently reported permanent molecular doping technique. Measurements at two National Metrology Institutes confirm accurate resistance quantisation below 5 nΩ Ω⁻¹. Furthermore, samples show no significant drift in carrier concentration and performance on multiple thermal cycles over three years. This development paves the way for dissemination of primary resistance standards based on epigraphene.