We report on the sensing stability of quantum nanosensors in aqueous buffer solutions for the two detection schemes of quantum decoherence spectroscopy and nanoscale thermometry. The electron spin properties of single nitrogen-vacancy (NV) centers in 25-nm-sized nanodiamonds have been characterized by observing individual nanodiamonds during a continuous pH change from 4 to 11. We have determined the stability of the NV quantum sensors during the pH change as the fluctuations of ±12% and ±0.2 MHz for the spin coherence time (T 2 ) and the resonance frequency (ω 0 ) of their mean values, which are comparable to the instrument error of the measurement system.We discuss the importance of characterizing the sensing stability during the pH change and how the present observation affects the measurement scheme of nanodiamond-based NV quantum sensing.

Surface oxidation of nanodiamonds (NDs) is a primary step of their surface functionalization that is key to the success of their recent emerging applications in nanoscale quantum sensors in biological samples. Here, we investigate how the electron spin coherence of single nitrogen vacancy centers in NDs is extended by two major oxidizing techniques, that is, aerobic oxidation and anaerobic triacid oxidation with various processing parameters. Aerobic oxidation at 550 °C most effectively oxidizes the surface and extends T 2 by a factor of 1.44 ± 0.33 to the original NDs. The ND size dependence of this T 2 extension shows that aerobic oxidation removes a constant decoherence contribution irrespective of the ND size, which clearly separates its origin from the surface-derived decoherence sources. The present results highlight the presence of the ND-specific decoherence sources other than surface termination spin noise and spin-active impurities, thereby improving the spin coherence of ND quantum sensors.

Capturing the fast rotational motion of single nanoparticles has been hindered owing to the difficulty of acquiring directional information under the optical diffraction limit. Here, we report the linewidth broadening of the electron spin resonance of single nitrogen vacancy (NV) centers that matches the rotational diffusion constant of the host nanodiamonds. When nanodiamonds are gradually detached from the substrates that they were fixed to, their optically detected spin resonance peaks are broadened by 1.8 MHz, which corresponds to the rotational diffusion constant of nanoparticles with a diameter of 11.4 nm from the Einstein–Smoluchowski relation.