Long Spin Relaxation Times in CVD-Grown Nanodiamonds

Abstract: Currently, the primary applications of fluorescent nanodiamonds (FNDs) are in the area of biosensing, by using photoluminescence or spin properties of colour centres, mainly represented by the Nitrogen Vacancy (NV) point defect. The sensitivity of NV-FNDs to external fields is, however, limited by crystallographic defects, which influence their key quantum state characteristics - the spin longitudinal (\textit{T$_1$}) and spin transversal (\textit{T$_2$}) relaxation and coherence times, respectively. We report on utilising an advanced FND growth technique consisting of heterogeneous nucleation on pre-engineered sites to create FNDs averaging around 60 nm in size, with mean longitudinal coherence times of 800 $μ$s and a maximum over 1.8 ms, close to bulk theoretical values. This is a major, nearly ten-fold improvement over commercially available nanodiamonds for the same size range of 50 to 150 nm. Heavy-N doped nanodiamond shells, important for sensing events in nm proximity to the diamond surface, are fabricated and discussed in terms of re-nucleation and twinning on {111} crystal facets. We also discuss scalability issues in order to enable the production of FND volumes matching the needs of sensing applications.