In this study, charge compensation was performed by co-doping Na + ions at the Ca2+ sites of Ce-doped LiCaAlF6 single crystals to prevent the generation of cation vacancies owing to Ce3+-doping at the Ca2+ sites. Consequently, an improved radiation resistance and increased light yield under neutron irradiation was achieved. In contrast, the Al metal of the starting material used as a substitute for AlF3 significantly increased the effective segregation coefficient keff of the Eu2+ ions in Eu-doped LiCaAlF6 and Eu-doped LiSrAlF6 single crystals. The Al metal and EuF3 in the starting materials produced EuF2 via a chemical reaction, and the Eu2+ ions in EuF2 could be substituted at the Ca2+ and Sr2+ sites. In addition, the Ca/Sr ratio control of the Li(Ca,Sr)AlF6:Eu solid-solution scintillator single crystals improved the light yield through band-gap control, and the Li(Ca,Sr)AlF6:Eu single crystal with a 25% Sr concentration exhibited the highest light yield.
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