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Fine‐tuning of graphene effective doping is achieved by applying ultrahigh pressures (>10 GPa) using atomic force microscopy (AFM) diamond tips. Specific areas in graphene flakes are irreversibly flattened against a SiO 2  substrate. This work represents the first demonstration of local creation of very stable effective p‐doped graphene regions with nanometer precision, as unambiguously verified by a battery of techniques. Importantly, the doping strength depends monotonically on the applied pressure, allowing a controlled tuning of graphene electronics. Through this doping effect, ultrahigh pressure modifications include the possibility of selectively modifying graphene areas to improve their electrical contact with metal electrodes, as shown by conductive AFM. Density functional theory calculations and experimental data suggest that this pressure level induces the onset of covalent bonding between graphene and the underlying SiO 2  substrate. This work opens a convenient avenue to tuning the electronics of 2D materials and van der Waals heterostructures through pressure with nanometer resolution.

Tunable Graphene Electronics with Local Ultrahigh Pressure