Observation of a Metastable Honeycomb Arrangement of C(60) on Ni(111) with (7 × 7) Periodicity: Tailoring an Interface for Organic Spintronics

[Image: see text] Hybrid nanostructures in which organic molecules are interfaced with metal surfaces hold promise for the discovery of intriguing physical and chemical phenomena, as well as for the development of innovative devices. In this frame, it is crucial to understand the interplay between the structural details of the interface and the electronic properties of the system. Here, an experimental investigation of the C(60)/Ni(111) interface is performed by means of scanning tunneling microscopy/spectroscopy (STM/STS) and low-energy electron diffraction (LEED). The deposition of C(60) at room temperature, followed by high-temperature annealing, promotes the stabilization of two different phases. A hitherto unreported phase forming a (7 × 7) honeycomb overlayer coexists with the well-known (4 × 4) reconstruction. Highly resolved STM images disclose the adsorption geometry of the molecules for both phases. STS reveals that the electronic properties of C(60)/Ni(111) are strongly influenced by the morphology of the interface, suggesting the possibility of tuning the electronic properties of the organic/inorganic heterostructures by adjusting the structural coupling with the substrate. This achievement can be important for hybrid magnetic interfaces, where the harmonization between the molecular and the magnetic orders can enhance the development of hybrid magnetic states.