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Fluorescent nanodiamonds (NDs) are crystal defect-based light-emittingnanoparticles that can be applied to quantum information science and quantumsensing. Of particular interest are nitrogen vacancy (NV) centers that allowoptical access to their coherently controllable electron spin systems, leadingto spin-photon quantum devices and nanoscale sensing of various physicalparameters. However, the NV spin coherence time (T2) in NDs has been limited toone or two orders of magnitude shorter than those in bulk diamonds owing to thecomplicated surface effect that decoheres the NV spin systems. Here, we studythe relation between the surface properties and T2 of single NV centers in NDsby systematically analyzing the effect of surface oxidation. We apply aerobicand acidic oxidation methods with various heating temperatures and processingtimes and find that aerobic oxidation most effectively oxidizes the surface andextends T2 by a factor of 1.6 to the original NDs. The ND-size dependence of T2clearly shows that the surface oxidation removes a constant decoherencecontribution irrespective of the ND size and that a new surface deriveddecoherence source emerges when the ND size reduces below 50 nm. The presentresults provide quantitative information on the decoherence sources of NV spinsystems of NDs and will enable a strategic surface modification for better spinmanipulations of NV centers in the context of quantum information science andnanoscale quantum sensing.

Effect of surface oxidation on electron spin coherence of single nitrogen-vacancy centers in nanodiamonds