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Journal of Alloys and Compounds

Modulating spin coherence time of NV− center ensembles in CVD diamond by low-pressure and high-temperature annealing

Qiuwen Dong, Y J, Sihan He, Shaoheng Cheng, Kuo Hu, Liuan Li, Zhaodong Liu, Hongdong Li, Bingbing Liu

Published Jun 29, 2026• 0 citations
Publisher
DOI
10.1016/j.jallcom.2026.189492

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We present the increase in the nitrogen vacancy center concentration in nitrogen delta-doped layers by almost one order of magnitude. To achieve this, we employ a low-pressure, high-temperature annealing step at 1750 °C in vacuum. We demonstrate an enhancement of the photoluminescence intensity of NV centers compared to annealing steps at lower temperatures of 1200 °C. To achieve this, we fabricate nitrogen-doped thin films with a thickness of 50 nm via chemical vapor deposition. We show that the nitrogen is mainly incorporated in a 6 nm thin film at the layer interface. We link the strong enhancement of the NV concentration to a possible decomposition of NVH centers and the mobility of various species at elevated temperatures, including vacancies and nitrogen in these two-dimensional structures. Additionally, after the high temperature annealing, we observe a Hahn-echo spin coherence time of 7.9 μ s, which is in line with literature data on achievable coherence time in highly nitrogen-doped layers. Our results could pave the way for the precise fabrication of improved diamond elements, e.g., used in magnetic field sensors and offer an alternative route to implantation techniques.
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 °C–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 °C–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 Δ ν ≈ 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 T 1 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.