authoren We have employed a range of atomistic simulation methods to explore aspects of defect chemistry in ABO3 (where A2+= Ba2+ or Sr2+, and B4+= Zr4+ or Hf4+) perovskites, placing emphasis on processes relevant for application of these materials as high performance scintillators. Specifically, we examined intrinsic defect reactions, A and B excess nonstoichiometry and the solution of Me3+ rare earth cations. As has been predicted in previous studies, we find that Schottky disorder is the lowest energy intrinsic process. For nonstoichiometry, we predict that AO‐excess is compensated by oxygen vacancies and BO2‐excess is charge compensated by A vacancies (see abstract figure). Finally, for Me3+ solution, we considered several reactions for Me3+ cations ranging in size from Lu3+ to La3+, and the preferred reaction depends on the specific Me3+ cation and whether or not phase separation occurs.
Nonstoichiometry mechanisms in ABO3 perovskites. Red spheres correspond to O2−, blue to A2+, and green to B4+.