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Diamond and Related Materials

Two types of stimulated emission in HPHT diamond with a high concentration of NV centers

Vyacheslav F. Lebedev, E. A. Vasilev, I.V. Klepikov, T.S. Misnikova, Ya. A. Ryvkina, A. V. Koliadin, Victor G. Vins

Published Nov 9, 2024• 10 citations
Publisher
DOI
10.1016/j.diamond.2024.111763

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Synthetic high-pressure high-temperature (HPHT) microdiamonds demonstrate strong resonant-like enhancement of the NV− photoluminescence (PL) at unexpectedly low concentration of the substitutional nitrogen atoms (NS) of 90 ppm, which is significantly smaller than the ∼250 ppm characteristic for conventional HPHT synthesis. The EPR, Raman, and luminescent spectroscopies, including time-resolved PL, provide evidence that this is due to competition between the increase in PL with increasing concentration of the NV− centers and nonradiative deactivation of these centers by defects induced by the NS in the diamond crystal lattice. It is suggested that the intensity of the NV− center emission can be optimized by the appropriate choice of nitrogen doping concentration which does not substantially disrupt the diamond crystal lattice.

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Since nitrogen-vacancy (NV) centers in diamond have emerged as crucial quantum sensors in physics and biology, the massive preparation of high-quality and high-concentration shallow NV center samples has become urgent and demanding. As NV centers approach the surface and their concentration increases, charge state instability can degrade coherence and introduce additional noise. This problem is further complicated in high-pressure and high-temperature (HPHT) diamonds due to the presence of unclear impurities and inhomogeneous strain. Through optically detected magnetic resonance testing on various implanted samples, we analyzed the spin and charge state properties of shallow NV center ensembles. Our results reveal that the doping dose significantly influences the quantity of NV−, charge, and charge stability. Our findings indicate that over-implanting nitrogen as electron donors before starting graphitization helps stabilize the charge environment of the shallow NV center ensembles. By controlling the nitrogen ion implantation dose, we optimized charge state stability under photoionization and prepared high-quality NV center ensemble samples in HPHT diamonds at the optimal implantation dose range of 2×1013–8×1013 ions/cm2. This method, which relies solely on nitrogen ion implantation and annealing on HPHT diamond, significantly reduces the cost of sensor samples, greatly benefiting the promotion of quantum sensing.
Synthetic high-pressure high-temperature (HPHT) microdiamonds demonstrate strong resonant-like enhancement of the NV− photoluminescence (PL) at unexpectedly low concentration of the substitutional nitrogen atoms (NS) of 90 ppm, which is significantly smaller than the ∼250 ppm characteristic for conventional HPHT synthesis. The EPR, Raman, and luminescent spectroscopies, including time-resolved PL, provide evidence that this is due to competition between the increase in PL with increasing concentration of the NV− centers and nonradiative deactivation of these centers by defects induced by the NS in the diamond crystal lattice. It is suggested that the intensity of the NV− center emission can be optimized by the appropriate choice of nitrogen doping concentration which does not substantially disrupt the diamond crystal lattice.