Ab initio electronic and optical properties of the N-V- center in diamond

Despite tremendous activity in employing the N-V- center in a host of quantum technology applications, the electronic and optical properties of the system are still not theoretically well understood. We have conducted density functional theory calculations of the N-V- system which show convergence at the 3×3×3 supercell level and for the first time produce a quantitatively accurate picture of the optical transition energy, excited-state lifetime, and optical polarization anisotropy taking into account all possible transitions within all contributing energy bands. These calculations were augmented by a group theoretical analysis, in sum providing a new ab initio understanding of this important solid-state quantum system.