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Charge transfer at the interface between dissimilar materials is at the heart of electronics and photovoltaics. Here we study the molecular orientation, electronic structure, and local charge transfer at the interface region of C 60 deposited on graphene, with and without supporting substrates such as hexagonal boron nitride. We employ ab initio density functional theory with van der Waals interactions and experimentally characterize interface devices using high-resolution transmission electron microscopy and electronic transport. Charge transfer between C 60 and the graphene is found to be sensitive to the nature of the underlying supporting substrate and to the crystallinity and local orientation of the C 60 . Even at room temperature, C 60 molecules interfaced to graphene are orientationally locked into position. High electron and hole mobilities are preserved in graphene with crystalline C 60 overlayers, which has ramifications for organic high-mobility field-effect devices.

Molecular Arrangement and Charge Transfer in C60/Graphene Heterostructures

Molecular Arrangement and Charge Transfer in C₆₀/Graphene Heterostructures