The NV−⋯N+ charged pair in diamond: a quantum-mechanical investigation

Abstract

The NV⁻⋯N⁺ charged pair in diamond has been investigated by using a Gaussian-type basis set, the B3LYP functional, the supercell scheme and the CRYSTAL code. It turns out that: (i) when the distance between the two defects is larger than 6–7 Å, the properties of the double defect are the superposition of the properties of the individual defects. (ii) The energy required for the reaction NV⁰ + N_s → NV⁻ + N⁺ is roughly −1.3 eV at about 12 Å, irrespective of the basis set and functional adopted, and remains negative at any larger distance. (iii) These results support the observation of a charge transfer mechanism through a N_s → NV⁰ donation occurring in the ground state, through a tunnelling process, without irradiation. (iv) The IR spectrum of the two subunits is characterized by specific peaks, that might be used as fingerprints. (v) Calculation of electrostatic interaction permitted an estimate of the effective charge of the defects.