DFT calculation of ²²⁹thorium-doped magnesium fluoride for nuclear laser spectroscopy

The ²²⁹thorium nucleus has an extremely low-energy isomeric state that could be manipulated with light in the vacuum ultraviolet (VUV) range. Recent measurements based on internal conversion electrons place the isomer energy at 8.28(17) eV (Seiferle B et al 2019), within the transmission window of large-band-gap materials, such as fluoride single crystals. Doping ²²⁹Th into VUV-transparent materials realizes a spectroscopy target with a high nuclei density and might form the basis of a solid-state nuclear clock. This paper presents a theoretical study of the optical properties of a thorium-doped MgF₂ crystal. Using the Vienna Ab-initio Simulation Package, we perform density functional theory calculations of the electronic and optical properties of Th:MgF₂. We determine whether thorium will be accepted as a dopant and identify the charge compensation mechanism and geometry. The simulations indicate, that the band gap of Th-doped MgF₂ will be significantly reduced compared to undoped MgF₂, below the expected ²²⁹Th isomer energy. This result is in striking contrast to a similar study performed for Th-doped CaF₂ (Dessovic P et al 2014 J. Phys. Condens. Matter 26 105402).