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Tuning the charge carrier density of two-dimensional (2D) materials byincorporating dopants into the crystal lattice is a challenging task. Anattractive alternative is the surface transfer doping by adsorption ofmolecules on 2D crystals, which can lead to ordered molecular arrays. However,such systems, demonstrated in ultra-high vacuum conditions (UHV), are oftenunstable in ambient conditions. Here we show that air-stable doping ofepitaxial graphene on SiC - achieved by spin-coating deposition of2,3,5,6-tetrafluoro-tetracyano-quino-dimethane (F4TCNQ) incorporated in poly(methyl-methacrylate) - proceeds via the spontaneous accumulation of dopants atthe graphene-polymer interface and by the formation of a charge-transfercomplex that yields low-disorder, charge-neutral graphene with carriermobilities ~70,000 cm2/Vs at cryogenic temperatures. The assembly of dopants on2D materials assisted by a polymer matrix, demonstrated by spin coatingwafer-scale substrates in ambient conditions, opens up a scalable technologicalroute towards expanding the functionality of 2D materials.

Uniform doping of graphene close to the charge neutrality point by polymer-assisted spontaneous assembly of molecular dopants