Graphene‐Based Heterostructured Arrays with Tunable Bandgap: A General and Forsaken Strategy

Abstract The pristine graphene is being subjected to zero bandgap and low charge carrier density in nanoelectronic and optoelectronic fields. Designing a versatile platform, constructing perfect interface, and understanding the interface physics in graphene‐based hybrids or heterostructures have therefore been one of the most effective paths for applications in foreseeable future. Unfortunately, inhomogeneous chemical composition and weak interface exert unfavorable effects on such systems because graphene tends to irreversibly restack and subside in solutions. Here, a general method for the preparation of Nb₃O₇F array/graphene (NOFA/G) heterostructures is demonstrated utilizing defect‐chemical technique, homogeneous nucleation, and preferential growth. As a distinguishing method, the solution process is an important scalable approach through oxyfluorinated functionalization on the basal plane of graphene. In particular, constructing NOF arrays on graphene platform markedly enhances light‐harvesting capacity. Moreover, the adsorption edge and bandgap can be effectively tuned according to the degree of oxyfluorinated functionalization. This general strategy extends the preparation of oxyfluoride array/carbon heterostructures and may open a door to other carbon‐based heterostructure, such as oxychloride array/carbon heterostructures, oxysulfide array/carbon heterostructures, etc.