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

The fluorescent nitrogen-vacancy (NV) defect in diamond has remarkable photophysical properties, including high photostability, which allows stable fluorescence emission for hours; as a result, there has been much interest in using nanodiamonds (NDs) for quantum optics and biological imaging. Such applications have been limited by the complexity and heterogeneity of ND photophysics. Photophysics of the NV center in NDs have been studied before, but the lack of a sensitive and high-throughput method has limited the characterization of NDs. Here is reported a systematic analysis of NDs using two-color wide-field epifluorescence imaging coupled to high-throughput single-particle detection of single NVs in NDs with sizes down to 5-10 nm. By using fluorescence intensity ratios, the charge conversion of single NV center (NV- or NV0) is observed and the lifetimes of different NV charge states in NDs is measured. The discovery of reversible manipulation of NV charge states by pH is also presented. In addition to provide another mechanism to control the NV charge state in nanodiamonds, our findings open the possibility to perform pH nanosensing with a non-photobleachable probe.
Comment: Manuscript: 30 pages, 5 figures; supplementary information: 12 pages, 11 figures