Tuning of SiV quantum emission in nitrogen-doped nanodiamonds by dual-color excitation

The charge dynamics of silicon-vacancy (SiV) centers have been investigated for the first time in high-pressure high-temperature nanodiamonds (NDs) with varying concentrations of substitutional nitrogen (Ns). We demonstrate a controlled sixfold enhancement of SiV- photoluminescence (PL) under dual-color excitation, consisting of strong red (~660 nm) illumination combined with weak green (~530 nm) excitation. The measured dependencies of SiV- PL lifetime and intensity on excitation wavelength, together with the enhancement dependence on Ns concentration in the studied nanodiamonds, provide unambiguous evidence of the involvement of donor nitrogen in SiV-emission dynamics. Saturation curves and second-order PL intensity correlation measurements further indicate suppression of the population of the optically inactive SiV2- state upon the addition of green excitation. These results unlock a practical pathway toward engineering optically-controlled and scalable quantum emitters based on SiV-luminescent diamond nanoparticles.