Layer-by-layer construction of diamond devices for spin-sensing calls for atomistic understanding of the nitrogen species on diamond surfaces. As motivated by recent experiments using X-ray photoelectron spectroscopy and temperature-programmed desorption, we conducted density functional theory simulations to examine the adsorption and thermal evolution of the nitrogen species on the pristine and hydrogenated diamond(001) surfaces by nitrogen plasma. On the pristine diamond(001), we find that nitrogen species favor to attack the C=C dimers, forming nitrogen-dimers in a horizontal configuration, h-N2(ad). The formation of h-N2(ad) is capable of resolving some discrepancy in the literature. On the hydrogenated diamond(001), by contrast, there emerges a new state of nitrogen-dimers in a vertical configuration, v-N2(ad), in addition to h-N2(ad). Consequently, the desorption barriers of N2 is altered, i.e. Ea=0.91 eV on bare diamond(001) versus Ea=2.36 eV on hydrogenated diamond(001). Our findings demonstrate the role that surface hydrogenation plays in stabilizing nitrogen species adsorbed on diamond(001) by nitrogen plasma. Follow-up work on diamond(111) is currently underway.

Adsorption and thermal evolution of nitrogen species on pristine and hydrogenated diamond surfaces: A comparative study

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ACS Fall 2022

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