Long-Lived Ensembles of Shallow NV^- Centers in Flat and Nanostructured Diamonds by Photoconversion

Shallow, negatively charged nitrogen-vacancy centers (NV^-) in diamond have been proposed for high-sensitivity magnetometry and spin-polarization transfer applications. However, surface effects tend to favor and stabilize the less useful neutral form, the NV⁰ centers. Here, we report the effects of green laser irradiation on ensembles of nanometer-shallow NV centers in flat and nanostructured diamond surfaces as a function of laser power in a range not previously explored (up to 150 mW/μm²). Fluorescence spectroscopy, optically detected magnetic resonance (ODMR), and charge-photoconversion detection are applied to characterize the properties and dynamics of NV^- and NV⁰ centers. We demonstrate that high laser power strongly promotes photoconversion of NV⁰ to NV^- centers. Surprisingly, the excess NV^- population is stable over a timescale of 100 ms after switching off the laser, resulting in long-lived enrichment of shallow NV^-. The beneficial effect of photoconversion is less marked in nanostructured samples. Our results are important to inform the design of samples and experimental procedures for applications relying on ensembles of shallow NV^- centers in diamond.