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The fluorescent nitrogen-vacancy (NV) defect in diamond has remarkablephotophysical properties, including high photostability, which allows stablefluorescence emission for hours; as a result, there has been much interest inusing nanodiamonds (NDs) for quantum optics and biological imaging. Suchapplications have been limited by the complexity and heterogeneity of NDphotophysics. Photophysics of the NV center in NDs have been studied before,but the lack of a sensitive and high-throughput method has limited thecharacterization of NDs. Here is reported a systematic analysis of NDs usingtwo-color wide-field epifluorescence imaging coupled to high-throughputsingle-particle detection of single NVs in NDs with sizes down to 5-10 nm. Byusing fluorescence intensity ratios, the charge conversion of single NV center(NV- or NV0) is observed and the lifetimes of different NV charge states in NDsis measured. The discovery of reversible manipulation of NV charge states by pHis also presented. In addition to provide another mechanism to control the NVcharge state in nanodiamonds, our findings open the possibility to perform pHnanosensing with a non-photobleachable probe.

High-Throughput Detection and Manipulation of Single Nitrogen-Vacancy Center's Charge in Nanodiamonds