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The chemical functionalization of graphene enables control over electronicproperties and sensor recognition sites. However, its study is confounded by anunusually strong influence of the underlying substrate. In this paper, we showa stark difference in the rate of electron transfer chemistry with aryldiazonium salts on monolayer graphene supported on a broad range of substrates.Reactions proceed rapidly when graphene is on SiO_2 and Al_2O_3 (sapphire), butnegligibly on alkyl-terminated and hexagonal boron nitride (hBN) surfaces. Theeffect is contrary to expectations based on doping levels and can instead bedescribed using a reactivity model accounting for substrate-inducedelectron-hole puddles in graphene. Raman spectroscopic mapping is used tocharacterize the effect of the substrates on graphene. Reactivity imprintlithography (RIL) is demonstrated as a technique for spatially patterningchemical groups on graphene by patterning the underlying substrate, and isapplied to the covalent tethering of proteins on graphene.

Chemical reactivity imprint lithography on graphene: Controlling the substrate influence on electron transfer reactions