High quantum yield luminescence and scintillation properties of high-Ce-doped MgF2-Al2O3-B2O3 glasses and their glass structure

Ce-doped inorganic single crystals are currently used in scintillators in various instruments because of their outstanding luminescence properties. However, these crystals are expensive to manufacture and are inefficient in terms of their energy consumption. In this study, xCeF(3)-doped 40MgF(2)-20Al(2)O(3)-40B(2)O(3) glasses (x = 0-30 mol%) were prepared by a melt-quenching method in N-2 atmosphere, and their photoluminescence, scintillation, and dosimetry properties were investigated. The X-ray absorption fine edge spectroscopy of the Ce L-3-edge indicated that the doped Ce exists in the form of Ce3+ ions, and that Ce4+ does not form because of the low basicity of the glass. The glasses underwent photoluminescence at 380 nm due to the 5d-4f transition of Ce3+, with a very high quantum yield of up to similar to 100 % and low concentration quenching. The peak shape of the X-ray-induced luminescence was similar to that of the PL with a decay time of 110-70 ns. The light yields for gamma rays (Cs-137 source) were obtained from the pulse-height spectra, and the highest light yield among the present samples was 1071 photons/MeV with the energy resolution of 17 %. The thermoluminescence glow curves had peaks at 365 and 460 K and a good linear relationship existed in the range of 0.5-1000 mGy, with the dose response being comparable to that of a commercial dosimeter. The origin of the high quantum yield was probed by analyzing the glass structure using molecular dynamics simulation based on a graph neural network. A strong tendency to selectively bind cations and anion pairs was found: Mg preferably binds to F, B preferably binds to O, and Al binds to O and F, which can be explained by soft and hard acid and base theories. Because of this selectivity the glass forms fluoride- and oxide-rich domains, which seem to be responsible for the more effective dispersal of the luminescent center. The results of this study are expected to contribute to the development of glasses with enhanced photoluminescence and scintillation luminescence properties.