Enhanced photoluminescence quantum yield of Ce³⁺‐doped aluminum–silicate glasses for scintillation application

Abstract

Ce3+‐doped 20Gd2O3–20Al2O3–60SiO2 (GAS:xCe3+) glasses (x = 0.3, 0.7, 1.1, 1.5, 1.9 mol%) with Si3N4 as a reducing agent were prepared. The density of the glasses is around 4.2 g/cm3. With the increase in the Ce3+ concentration, both the photoluminescence (PL) and PL excitation peaks of GAS:xCe3+ glasses show a redshift because the 4f–5d energy levels of Ce3+ ions are narrowed. PL quantum yield and PL decay time of GAS:xCe3+ glasses are 28.32–50.59% and 43–64 ns, respectively. In addition, they both first increases and then decreases with the Ce3+ concentration increasing, reached the maximum when x = 1.1 mol%. The integrated X‐ray excited luminescence (XEL) intensity of the GAS:1.1Ce3+ glass is 23.86% of that of Bi4Ge3O12 (BGO) crystal, and the light yield reaches 1200 ph/MeV with an energy resolution of 22.98% at 662 keV when exposed to γ‐rays. The PL and XEL thermal activation energies of GAS:xCe3+ glasses are independent of Ce3+ ions concentration. Scintillating decay time of the glasses exhibits two components consisting of nanosecond and microsecond levels, and the scintillating decay time gradually decreases with the Ce3+ concentration increasing. The difference between PL and scintillating decay time is discussed regarding the different luminescent mechanisms.

Band Gap and Defect Engineering Enhanced Scintillation from Ce3+-Doped Nanoglass Containing Mixed-Type Fluoride Nanocrystals

“…The scintillation decay can be fitted by a double-exponential function consisting of two components (Figure (d)), a fast (∼0.075 μs, 70%) and a slow (∼0.743 μs, 30%) one. The RL decay is longer than the PL one (Figure (c)) and can be accounted for by the trap-delayed ET in Gd 3+ -mixed scintillators. ,, Further improvement in time response as well as in LY will be made possible via optimization of the Y 3+ –Gd 3+ mixing ratio, Ce 3+ concentration, and the use of aliovalent doping as well as heterostructures . Sidletskiy et al found empirically that the optimal range of the ratio of ionic radii between substitution and host ions is 1.05–1.15 to realize the greatest improvement in LY …”

“…Moreover, they are confronted with the difficulty in mechanical processing and are particularly incompatible with the conventional fiber-drawing technique . In lieu of crystals, Ce 3+ -doped glasses have been extensively explored, thanks to their much lower production cost (about one-thirtieth of the BGO crystal), simpler processing, and being more adapted to commercialization. , Scintillator glasses are notably favorable for making large-volume detectors for future particle collider experiments (e.g., the Circular Electron Positron Collider in China). Besides, with the surging demand for oil well logging, gas exploration, and safety concerns on nuclear proliferation, the global market size is very encouraging for bulk scintillator glasses and optical fibers (with an anticipated compound annual growth rate of 4.01% from 2022 to 2027).…”

“…Besides, with the surging demand for oil well logging, gas exploration, and safety concerns on nuclear proliferation, the global market size is very encouraging for bulk scintillator glasses and optical fibers (with an anticipated compound annual growth rate of 4.01% from 2022 to 2027). However, because charge carriers tend to be trapped by many defective sites in an amorphous matrix, most glasses (especially those with large densities, d ≥ 5.0 g/cm 3 ) suffer from a relatively low LY (<1000 ph/MeV) and a poor ER (>20%) (Table S1, Supporting Information). Consequently, only a few brands of glasses (e.g., Ce 3+ -doped lithium aluminosilicate glass, GS20) are available in the market and utilized mainly in thermal neutron detection (due to a low density of 2.5 g/cm 3 ).…”

“…However, because charge carriers tend to be trapped by many defective sites in an amorphous matrix, most glasses (especially those with large densities, d ≥ 5.0 g/cm 3 ) suffer from a relatively low LY (<1000 ph/MeV) and a poor ER (>20%) (Table S1, Supporting Information). Consequently, only a few brands of glasses (e.g., Ce 3+ -doped lithium aluminosilicate glass, GS20) are available in the market and utilized mainly in thermal neutron detection (due to a low density of 2.5 g/cm 3 ). To enhance the LYs of glasses, energy transfer sensitization based on nearly resonant energy migration through the Gd 3+ sublattice followed by a single-step transfer to Ce 3+ has been used (strategy I, Figure 1(c)).…”

All‐Inorganic Glass Scintillators: Scintillation Mechanism, Materials, and Applications

“…[51] At present, the commonly employed in glass scintillators are Ce 3+ , Tb 3+ and Eu 3+ , which are directly doped into glass matrix or doped into micro/nano crystals embedded in glass. [28,[54][55][56][57][58][59][60][61] The electronic configuration of rare earth elements can be written as [Xe]4f 0-14 5d 0-1 6s 2 . In accordance with the parity selection rules, also referred to as Judd-Ofelt theory, [62] electric dipole transition is only feasible between different parity states.…”