The effect of Ga‐doping on the defect chemistry of RE₃Al₅O₁₂ garnets

Abstract

Abstract It has been recently shown that the addition of Ga to Lu 3 Al 5 O 12 garnet (LuAG) removes the electron trapping associated with cation antisite defects. In this paper, we show via atomic scale simulations that the replacement of Al with Ga in LuAG actually lowers the energy of the antisite disorder process. Thus, we predict that Ga additions will lead to an increase of the antisite defect concentration and, in the absence of the electronic structure changes, would actually degrade the performance of the material. Since there are two crystallographically distinct Al sites in the garnet structure, we not only present results for complete replacement of Al with Ga, but also partial replacement for 40% (on 16a) and 60% (on 24d) of the Al with Ga. Our results support the explanation for Ga‐doping leading to improvement in garnet scintillator performance that relies on variations of the electronic structure rather than reduction of the antisite defect concentration. magnified image Cation antisite defects in RE 3 Al 5 O 12 garnet, where small light gray atoms and large dark gray atoms are lattice Al and RE atoms, respectively. The constituents of the antisite defect pairs are labeled, and it should be noted that the Ga atom (blue) is similar in size to RE (green). Oxygen atoms are not shown for clarity.