High-Order Commensurate Zwitterionic Quinonoid Phase Induces a Nanoscale Dipole Lattice on Graphene

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Since the introduction of hybrid van der Waals heterostructures (h-vdWHs) for device architecture development, many vertically staked organic two-dimensional materials have been investigated in order to control transport properties. This article introduces a novel h-vdWH that achieves periodic interaction by the development of a superlattice. We describe a complete investigation of the diphenyl-functionalized p-benzoquinonemonoimine zwitterion on highly oriented pyrolytic graphite and monolayer graphene using high-resolution scanning tunneling microscopy images and numerical simulations. The molecular phase on both substrates exhibits a structurally identical antiparallel dipole alignment in a head-to-tail dimer configuration. Density functional theory calculations reveal that this molecular adsorption induces a local dipole at the graphene interface due to the rearrangement of the electron density distribution.