Enhancing the yield and concentration of colour centres in diamonds is crucial for boosting their quantum field applications. Although nitrogen impurities in diamond play an important role in the formation of nitrogen-related (NV and H3) colour centres, the effect of the concentration and form of nitrogen impurities on the formation of nitrogen-related centres in diamonds is not yet clear. To effectively address this problem, in this work, single-crystal diamonds with various nitrogen contents (0 to 760 ppm) under high-pressure and high-temperature conditions were synthesized. An annealing process was also implemented under the application of 3.5 GPa pressure and within temperatures ranging from 1,600 to 1,950 °C. The formation of NV and H3 centres was systematically investigated using low-temperature photoluminescence spectroscopy. The results showed that annealing diamonds of type IIa with nitrogen content <1 ppm resulted in the simultaneous formation of high-intensity H3, NV0, and NV− centres. Compared to others, the diamond containing approximately 80 ppm of nitrogen showed the highest intensity of NV− centres across all annealing temperatures. Furthermore, as the nitrogen content exceeded 80 ppm, the intensity of the NV− centres gradually declined, and when the nitrogen content was 760 ppm, only a trace amount NV− centres was produced. In addition, a large amount of C-centre nitrogen aggregated to form A-centre nitrogen during annealing, increasing the possibility of nitrogen forming Ni-N-related colour centres, thereby hindering the formation of NV and H3 centres. However, by electron irradiation of high-nitrogen-content diamond, we also obtained high-intensity and high-concentration NV− centres, and did not form Ni-N-related centres. Our work provides valuable insights for better understanding and optimizing the generation of NV and H3 centres in diamonds.
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