4.7 Article

Characterization of the nitrogen state in HPHT diamonds grown in an Fe-C melt with a low sulfur addition

Journal

CRYSTENGCOMM
Volume 24, Issue 24, Pages 4408-4416

Publisher

ROYAL SOC CHEMISTRY
DOI: 10.1039/d2ce00487a

Keywords

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Funding

  1. Ministry of Science and Higher Education of the Russian Federation [075-15-2020-781]

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This paper reports the results of growing diamonds in an Fe-C melt with the addition of 1% sulfur under high-pressure high-temperature conditions. It was found that adding 1% sulfur can significantly reduce the concentration of nitrogen defects in diamonds, resulting in near-colorless diamonds. The analysis of intense photoluminescence confirms that nitrogen impurities in diamonds mainly exist as single substitutional atoms.
This paper reports the results of high-pressure high-temperature (HPHT) diamonds growing in an Fe-C melt with introduction of 1 wt% sulfur. Experiments were carried out at a pressure of 6.0 GPa and a temperature of 1450 degrees C. It was found that adding 1 wt% sulfur leads to a significant decrease in the concentration of nitrogen defects in diamonds. As a result, the grown diamonds are near-colorless containing nitrogen in the range of 20-40 ppm. The dominant state of nitrogen impurities in the form of single substitutional atoms was confirmed by intense photoluminescence arising from the nitrogen-vacancy complexes in different charge states (NV0 and NV-). Only a very small number of nitrogen atoms are present as pairs (A and H3 centers). It is suggested that the pronounced effect of sulfur is attributed to the role of supercritical fluid in crystallization medium. Interaction between components of the H-O-C-S-N fluid leads to an increase in the proportion of complex hydrocarbons, including N-containing hydrocarbons. As a result, nitrogen atoms, which are present in the metal melt, are bound within the supercritical fluid. This nitrogen binding keeps dissociated nitrogen from entering the diamond structure.

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