Ab initiocalculation of hyperfine interactions for the5A2excited state of the neutral vacancy in diamond

We calculate the electronic properties and in particular the hyperfine interactions for the ${}^5{A}_2$ excited state of ${\mathrm{V}}_{\mathrm{C}}^0$ and for the unrelaxed ${}^4{A}_2$ ground state of ${\mathrm{V}}_{\mathrm{C}}^{-}$ in diamond. We find fair agreement with experimental electron paramagnetic resonance data for the hyperfine interactions of both defect states. Our results demonstrate that the local spin density approximation yields reliable magnetization densities, not only for the ground states but also for certain excited states of deep defects.