NV center emission in a substrate free low index environment

With in-built advantages (high quantum efficiency and room temperature photostability1) for deployment in quantum technologies as a bright on-demand source of single photons, the nitrogen vacancy (NV) center is the most widely studied optical defect in diamond. Despite significant success in controlling its spontaneous emission2, the fundamental understanding of its photo-physics in various environments and host material remains incomplete. Studying NV photoemission from nanodiamonds on a glass substrate, we recently pointed out a disparity between the measured and calculated decay rates (assuming near unity quantum efficiency)3. This indicates the presence of some strong nonradiative influences from factors most likely intrinsic to nanodiamond itself. To obtain a clearer picture of the NV emission, here we remove the substrate contributions to the decay rates by embedding our nanodiamonds inside silica aerogel, a substrate-free environment of effective index n ∼ 1.05. Nanodiamond doped aerogel samples were fabricated using the two-step process4. Time-resolved fluorescence measurement on ∼20 centers for both coverslip and aerogel configurations, showed an increase in the mean lifetime (∼37%) and narrowing of the distribution width (∼40%) in the aerogel environment, which we associate with the absence of a air/cover-glass interface near the radiating dipoles3. Finite difference time domain (FDTD) calculations showed the strong influence of the irregular nanodiamond geometry on the remaining distribution width. Finally a comparison between measurements and calculations provides an estimate of the quantum efficiency of the nanodiamond NV emitters as ∼0.7. This value is apparently consistent with recent reports concerning the oscillation of the NV center between negative and neutral charge states5.