DATA: Interaction between shallow NV− and spin active azafullerenes on hydrogenated and fluorinated (001) diamond surfaces.

The interaction between surface-lying nitrogen-substituted fullerenes (radical azafullerene, C59N[•]) with sub-surface negative nitrogen-vacancy complexes (NV[−]) in diamond is investigated using first principles calculations. We consider (2×1) reconstructed (001) oriented diamond surfaces with both H- and F-surface termination. The charge stability of NV[−] when in close proximity to both the nearby surface and the spin active azafullerene is discussed, in the context of diamond band bending arising from surface-induced changes in electron affinity (EA). In the case of the hydrogenated surface, the system spin is quenched, yielding a negatively charged azafullerene (C59N[−]) and neutrally charged NV[0] as the most stable electronic configuration. In contrast, fluorinating the surface favours the negatively charged NV[−] and conserves the C59N[•] neutrality and stabilizes uncompensated free spins. This opposing behaviour is attributed to surface charge doping emerging from different band bending effects associated with the surface EA. This study is consistent with experimentally observed photoluminescence quenching, and shows that surface passivation by fluorination could efficiently tackle the problem of charge transfer between adsorbed molecules and shallow NV centers.