Functionalized Fluorescent Nanodiamonds with Millisecond Spin Relaxation Times

Fluorescent nanodiamonds (FNDs) containing nitrogen-vacancy (NV) defects are useful probes for biological imaging and nanoscale sensing applications. Here, we explore the effect of chemical surface modifications and core–shell structures on the T1 relaxation times of 100 nm FNDs hosting nitrogen-vacancy ensembles. The results show that surface oxidation and silica coating of FNDs using the Stöber method can dramatically increase the spin relaxation time from T1 = 320 ± 9 μs to T1 = 1.00 ± 0.06 ms. Using FT-IR and NEXAFS measurements conducted on air oxidized particles, we find that changes to surface functional groups and sp2 carbon density may be responsible for the observed enhancements to the spin relaxation rate. Finally, we use a Monte Carlo model to numerically investigate the relationship between chemical sensitivity and shell thickness and find that a shell thickness on the order of 1 nm should provide the highest sensitivity. Our findings demonstrate that the surface of FNDs can be engineered to exhibit bulk-like T1 relaxation times, in the absence of complex quantum control sequences, which is crucial to advancing biosensing and imaging applications where surface spin noise currently limits measurement precision.