The zero-dimensional all-inorganic perovskites are self-activated blue emitters with slight hygroscopicity, scalable synthesis, and high radiation detection efficiency.

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Lithium codoping has emerged as an effective strategy to enhance the light yield of oxide scintillators for radiation detection applications, but the understanding of the actual role played by Li+ remains unclear. In this work, we comprehensively study the effects of Li codoping on optical and scintillation properties of Lu2SiO5:Ce (LSO:Ce) single crystals and reveal the critical role of site occupancy of Li. High-quality LSO:Ce single crystals codoped with 0.05, 0.1, and 0.3 at. % Li ions were grown by the Czochralski method. The optical absorption spectra confirm nonconversion of stable Ce3+ to Ce4+ in Li-codoped LSO:Ce regardless of the Li codoping concentration. The photoluminescence decay kinetics suggest an enhanced ionization of the excited 5d1 state of Ce3+ centers in highly codoped samples. A simultaneous improvement of scintillation light yield, decay time, and afterglow is achieved in LSO:Ce codoped with low concentrations of Li. The preferential occupation of Li at interstitial spaces and lutetium sites is proven to rely on its codoping concentration by using the 7Li nuclear magnetic resonance technique. The concentration-dependent site occupancy of Li alters the defect structures of LSO:Ce, in particular resulting in a distinct change in the number of cerium spatially correlated oxygen vacancies confirmed by thermoluminescence and afterglow measurements.