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Nitrogen is successfully doped in diamond by adding sodium azide (NaN3) as the source of nitrogen to the graphite and iron powders. The diamond crystals with high nitrogen concentration, 1000-2200 ppm, which contain the same concentrations of nitrogen with natural diamond, have been synthesized by using the system of iron-carbonadditive NaN3. The nitrogen concentrations in diamond increase with the increasing content of NaN3. When the content of NaN3 is increased to 0.7-1.3 wt.%, the nitrogen concentration in the diamond almost remains in a nitrogen concentration range from 1250 ppm to 2200 ppm, which is the highest value and several times higher than that in the diamond synthesized by a conventional method without additive NaN3 under high pressure and high temperature (HPHT) conditions.