Technological factors and processes contributing to the scintillation mechanism have been considered in quaternary garnet ceramics doped with Ce(Gd,Lu)3Al2Ga3O12. The super-stoichiometric additive of gadolinium in the material composition or its co-doping with a low concentration of Mg were found to be effective tools to suppress phosphorescence in the quaternary garnet, confirming that it is not an intrinsic property of the material. The Monte-Carlo simulation of electronic excitation transfer demonstrates that the hopping migration along the gadolinium sublattice plays an essential role in forming the scintillation kinetic parameters. Breaking the integrity of the gadolinium sublattice by substitution with heavier lutetium ions increases the role of self-trapped states in the excitation of Ce3+ ions, which ensures both an increase in the fraction of short ~20 ns and very long ~600 ns components in the scintillation kinetics.
A method to create compositionally disordered compounds with a high number of cations in the matrices, that utilize the cubic spatial symmetry of the garnet-type crystalline systems is demonstrated. Mixtures of the garnet-type powdered materials solely doped with Ce were used to create atomic compositions of high complexity. Several mixed systems, namely Gd3Al2Ga3O12/(Gd,Y)3Al2Ga3O12, Y3Al5O12/Gd3Al2Ga3O12, and Y3Al5O12/Y3Al2Ga3O12 were annealed, compacted and sintered in air. The materials were evaluated for structural, luminescence, and scintillation properties. It was demonstrated that the properties of the resulting ceramics are a little dependent on the granularity of powders when the median particle size is below ~5 μm.
The production of scintillating ceramics can require the utilization of the phosphorus compounds at certain stages of 3D-printing, such as vat polymerization, applied for the formation of green bodies before sintering. The effect of phosphorus additive on the microstructure, optical, and scintillation parameters of Gd1.494Y1.494 Ce0.012Al2Ga3O12 (GYAGG:Ce) ceramics obtained by pressureless sintering at 1650 °C in an oxygen atmosphere was investigated for the first time. Phosphorus was introduced in the form of NH4H2PO4 into the initial hydroxycarbonate precipitate in a wide concentration range (from 0 to 0.6 wt.%). With increasing of phosphorus concentration, the density and the optical transmittance of garnet ceramics show a decrease, which is caused by an increase in the number of pores and inclusions. The light yield of fast scintillation, which is caused by Ce3+ ions, was found to be affected by the phosphorus additive as well. Moreover, an increase in phosphorescence intensity was recognized.
The technological aspects of the light inorganic crystalline compounds suitable to create scintillation materials to detect charged particles and neutrons in a wide energy range have been examined. Among them, Li2CaSiO4:Eu was found to be a prospective candidate to control the valent state of the Rare Earth (RE) and to provide a high intensity of luminescence. It was demonstrated that the material has room for future improvement; however, this requires precise engineering of its composition—an experimental search of compositions or additives that will provide the maximum Eu2+/Eu3+ ratio to achieve a high scintillation light yield. The benefits of light inorganic materials are disclosed through the modeling of the linear density of nonequilibrium carriers along secondary particle tracks created in scintillators utilized for neutron detection. It is shown that oxide matrices have a larger linear density in comparison with halide crystalline compounds under alpha-particles and tritons, whereas light oxides can provide smaller numbers under protons.
New scintillation transparent ceramics Y3Al2.5Ga2.5O12:Ce, Mg has been produced and evaluated for the first time. The material possesses a density of 5.17 g/cm3, a highlight yield of 44,000 ph/MeV, and an effective scintillation kinetics decay constant of 47 ns. This unique combination of the parameters makes it superior to YAG:Ce. Production of the material does not include tooling from precious materials, and the rate of the crystalline mass production is not limited by the pulling rate of the crystal growth process. It can be quite prospective to upgrade the detection units of a variety of X-ray imaging devices. The mechanism of the scintillation light yield enhancement and kinetics shortening in the material are discussed as well.
Compositionally disordered crystalline material (Gd,Y,Tb,Ce)3Al2Ga3O12 was demonstrated to be a highly effective converter of corpuscular ionizing radiation into light. The material was found to be radiation-tolerant to an intense 10 MeV electron beam and had a low temperature dependence on light yield. These findings open an opportunity to utilize the developed material to create long-living, high-flux sources of optical photons under the irradiation of isotope sources. Besides the purposes of the measurement of ionizing radiation by the scintillation method in a harsh irradiation environment, this puts forward the exploiting of the developed material for indirect isotope voltaic batteries and the consideration of a photon engine for travel beyond the solar system, where solar wind force becomes negligible.