Optimizing Ensemble NV-Spin Properties of Fluorescent Diamond Microparticles by Systematic Low Pressure High Temperature Annealing

Nicholas Nunn^1*Antonin Marek^1,2Marco D. Torelli¹Alex I. Smirnov³Olga A. Shenderova^1*

• ¹Adamas Nanotechnologies, Inc., Raleigh, United States
• ²NC State University, Raleigh, United States
• ³Department of Chemistry, North Carolina State University, Raleigh, United States

Low pressure high temperature annealing is a means for driving nitrogen and defect diffusion in diamond to reduce internal lattice damage without the need for technically complicated high-pressure cells. Herein, we perform a systematic time (5, 15, and 30 min) and temperature (1200 – 1800 °C) study of effects of low-pressure high temperature annealing on photoluminescence, spin concentrations, and spin relaxation properties of NV centers in ca. 3 µm synthetic type 1b diamond particles. Annealing in the temperature range of ca. 1400 -1700 °C for even 5 min leads to a higher optically detected magnetic resonance contrast as compared to standard annealing at 900 °C for 2 h. Particles annealed at 1700 °C for 5 min exhibit a contrast close to about 13% as compared to about 9% for those annealed at 900 °C for 2 h. A reduction in the zero-field splitting strain parameter from E≈ 4.5 MHz to ≈ 2.5 MHz and spectral linewidth from Δ𝜈 ≈ 7 MHz to ≈ 4 MHz are observed even after 5 min annealing at 1700 °C. Improvements in these spectral parameters resulted in a roughly 2-fold reduction in the noise level of temperature monitoring experiment utilizing an ensemble of NV centers in the particles. Annealing in the temperature range of 1600 °C for 15 or 30 min or 1700 °C for 5 min resulted in NV T1 relaxation times approaching ca. 5 ms typically observed for bulk diamond. Quantitative electron paramagnetic resonance (EPR) allowed for estimations of thermal activation energies of paramagnetic center annihilation. Monitoring the primary defect concentration (P1 and other defects with half integer spins) and utilizing second order kinetic modeling, an activation energy of 3.63 ± 0.28 eV was estimated. Alternatively, using the NV half field EPR signal and first order kinetic modeling, a similar activation energy 3.89 ± 0.29 eV was estimated.