A microwave-assisted spectroscopy technique for determining charge state in nitrogen-vacancy ensembles in diamond.

We present a microwave-assisted spectroscopy technique for determining the relative concentrations of nitrogen vacancy (NV) centers in diamond that are negatively-charged (NV${}^-$) and neutrally-charged (NV${}^0$). Our method is based on selectively modulating the NV${}^-$ fluorescence with a spin-state-resonant microwave drive to isolate, in-situ, the spectral shape of the NV${}^-$ and, subsequently, NV${}^0$ contributions to an NV-ensemble sample's fluorescence. The sample-specific nature of this method accounts for any sample-to-sample variations in the spectral shape of the NV${}^-$ and NV${}^0$ fluorescence; and permits the investigation of the effect of material parameters, such as local strain and nitrogen concentration, on the steady-state charge-state distribution in NV ensembles. Our method does not rely on a specific illumination sequence, and can be applied with any illumination conditions of interest, as long as they produce fluorescence contrast between the NV${}^-$ spin states. The techniques presented here may be generalized to determine relative concentrations of other solid-state defects whose fluorescence can be selectively modulated by means of a microwave drive.