Point-defect optical transitions and thermal ionization energies from quantum Monte Carlo methods: Application to the F-center defect in MgO

Abstract

We present an approach to calculation of point-defect optical and thermal ionization energies based on the highly accurate quantum Monte Carlo methods. The use of an inherently many-body theory that directly treats electron correlation offers many improvements over the typically employed density functional theory Kohn-Sham description. In particular, the use of quantum Monte Carlo methods can help overcome the band-gap problem and obviate the need for ad hoc corrections. We demonstrate our approach to the calculation of the optical and thermal ionization energies of the F-center defect in magnesium oxide, and obtain excellent agreement with experimental and/or other high-accuracy computational results.