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

TL;DR

This study uses first principles calculations to explore how surface chemistry influences the charge stability and spin interactions between azafullerenes and NV centers in diamond, revealing surface passivation effects.

Contribution

It demonstrates how surface fluorination stabilizes NV$^-$ centers and preserves spin states, providing insights into controlling charge transfer in diamond-based quantum systems.

Findings

Hydrogenated surfaces quench NV$^-$ spin states.

Fluorinated surfaces favor NV$^-$ stability and free spins.

Surface passivation affects charge transfer and photoluminescence.

Abstract

The interaction between surface-lying nitrogen-substituted fullerenes (radical azafullerene, C$_{59}$N$^\bullet$) with sub-surface negative nitrogen-vacancy complexes (NV$^-$) in diamond is investigated using first principles calculations. We consider (2$\times$1) reconstructed (001) oriented diamond surfaces with both H- and F-surface termination. The charge stability of NV$^-$, when in close proximity to both the nearby surface and the spin active azafullerene is discussed, in the context of diamond band bending arising from surface-induced changes in electron affinity (EA). In the case of the hydrogenated surface, the system spin is quenched, yielding a negatively charged azafullerene (C$_{59}$N$^-$) and neutrally charged NV$^0$ as the most stable electronic configuration. In contrast, fluorinating the surface favours the negatively charged NV$^-$, and conserves the C$_{59}$N$^\bullet$, 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.