Spin-flip Bethe-Salpeter equation approach for ground and excited states of open-shell molecules and defects in solids

Abstract

Open-shell systems such as magnetic molecules or defects with a triplet ground state are challenging to describe in electronic structure methods, but are of great interest for quantum information applications. We demonstrate a spin-flip approach within the Bethe-Salpeter equation to calculate ground and excited states of open-shell molecules and defected solids. The approach works in periodic boundary conditions without any need for embedding or selection of a subspace. Our benchmark results for the torsion potential-energy surface of ethylene and the optical excitations of the diamond NV$^{-}$ center show excellent agreement with the literature, and a low or moderate level of spin contamination.