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Ultrahigh nitrogen-vacancy center concentration in diamond

High concentration of negatively charged nitrogen-vacancy ($\text{NV}^{-}$) centers was created in diamond single crystals containing approximately 100 ppm nitrogen using electron and neutron irradiation and subsequent thermal annealing in a stepwise manner. Continuous wave electron paramagnetic resonance (EPR) was used to determine the transformation efficiency from isolated N atoms to $\text{NV}^{-}$ centers in each production step and its highest value was as high as 17.5 %. Charged vacancies are formed after electron irradiation as shown by EPR spectra, but the thermal annealing restores the sample quality as the defect signal diminishes. We find that about 25 % of the vacancies form NVs during the annealing process. The large $\text{NV}^{-}$ concentration allows to observe orientation dependent spin-relaxation times and also the determination of the hyperfine and quadrupole coupling constants with high precision using electron spin echo (ESE) and electron-nuclear double resonance (ENDOR). We also observed the EPR signal associated with the so-called W16 centers, whose spectroscopic properties might imply a nitrogen dimer-vacancy center for its origin.