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Interaction between shallow NV− centers and spin-active azafullerenes on hydrogenated and fluorinated diamond (001) surfaces

Bastien Anézo*

Denis Arčon

Chris Ewels†

  • *Contact author: bastien.anezo@cnrs-imn.fr
  • †Contact author: chris.ewels@cnrs-imn.fr
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Phys. Rev. B 113, 045133 – Published 20 January, 2026

DOI: https://doi.org/10.1103/wphk-p6qb

Abstract

The interaction between surface-lying nitrogen-substituted fullerenes (radical azafullerene, C59N•) with subsurface 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 NV0 as the most stable electronic configuration. In contrast, fluorinating the surface favors 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.

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Phys. Rev. B 113, 045133– Published 20 January, 2026
  • Received 7 May 2025
  • Revised 25 September 2025
  • Accepted 22 December 2025
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