Synergistic Combination of Reductive Covalent Functionalization and Atomic Layer Deposition—Towards Spatially Defined Graphene‐Organic‐Inorganic Heterostructures

Abstract

AbstractThree‐dimensionally (3D) well‐ordered and highly integrated graphene hybrid architectures are considered to be next‐generation multifunctional graphene materials but still remain elusive. Here, we report the first realization of unprecedented 3D‐patterned graphene nano‐ensembles composed of a graphene monolayer, a tailor‐made structured organophenyl layer, and three metal oxide films, providing the first example of such a hybrid nano‐architecture. These spatially resolved and hierarchically structured quinary hybrids are generated via a two‐dimensional (2D)‐functionalization‐mediated atomic layer deposition growth process, involving an initial lateral molecular programming of the graphene lattice via lithography‐assisted 2D functionalization and a subsequent stepwise molecular assembly in these regions in the z‐direction. Our breakthrough lays the foundation for the construction of emerging 3D‐patterned graphene heterostructures.