Abstract
We report a breakthrough concept for a bulk single crystal as a heavy aluminum perovskite scintillator, where due to bandgap engineering by a balanced Gd admixture in a Lu cation sublattice, the scintillation performance dramatically increases. In an optimized composition of (Lu, Gd)AlO3:Ce (LuGdAP:Ce), the light yield approaches 21,000 phot/MeV, which is close to that of classical but much less dense YAP:Ce and 50% higher than the best LuYAP:Ce reported in the literature. Moreover, contrary to LuYAP:Ce, the LuGdAP host maintains a high effective atomic number close to that of LuAP:Ce (Zeff = 64.9), which is comparable to commercial LSO:Ce. An enormous decrease in afterglow on the millisecond time scale and acceleration in the rise time of the scintillation response further increase the application potential of the LuGdAP host. The related acceleration of the transfer stage in the scintillation mechanism due to diminishing electron trap depths is proven by thermally stimulated luminescence (TSL). Furthermore, we quantitatively characterize and model the energy transfer processes that are responsible for the change in the photoluminescence and scintillation decay kinetics of Ce3+ in the LuGdAP matrix. Such an innovative (Lu, Gd)AP:Ce scintillator will become competitive for use in applications that require heavy, fast, and high light yield bulk scintillators.
Highlights
Single crystal oxide-based scintillation materials are widely used in practical applications due to their mechanical and chemical stability and high performance[1,2]
Due to its low density and effective atomic number (Zeff), the R&D focus has oriented toward its heavy analog Lu3Al5O12:Ce (LuAG:Ce) and to multicomponent garnets based on the general formula (Lu,Y,Gd)3(Ga,Al)5O12:Ce5
The practical aspects, including the afterglow, scintillation rise, and decay on an extended dynamic time scale and light yield, were measured. All these results clearly showed that the bandgap engineering strategy and host optimization by the balanced Gd admixture in LuAP:Ce significantly accelerated the transfer of excitation energy toward the luminescent centers, sped up all the scintillation mechanism, and increased the light yield
Summary
Single crystal oxide-based scintillation materials are widely used in practical applications due to their mechanical and chemical stability and high performance[1,2]. Due to its low density and effective atomic number (Zeff), the R&D focus has oriented toward its heavy analog Lu3Al5O12:Ce (LuAG:Ce) and to multicomponent garnets based on the general formula (Lu,Y,Gd)3(Ga,Al)5O12:Ce (see the review)[5]. Ce garnet crystal matrix enables extended composition tailoring, which positively affects timing and efficiencyrelated scintillation characteristics[6,7,8,9]. This effect can be further enhanced by the stabilization of the Ce4+ center due to the stable divalent ion codoping reported in 201410. The positive effect of Ce4+ stabilization by Pokorný et al NPG Asia Materials (2021)13:66
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