Advances in Ce3+ doped Y1±xAlO3 (x≠0) single crystal perovskite scintillators through nonstoichiometric engineering

Q2 Engineering Optical Materials: X Pub Date : 2024-01-28 DOI:10.1016/j.omx.2024.100295

Karol Bartosiewicz , Jan Pejchal , Romana Kucerkova , Alena Beitlerova , Vladimir Babin , Vojtech Vanecek , Shunsuke Kurosawa , Kei Kamada , Akira Yoshikawa

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Abstract

The influence of nonstoichiometric engineering on the scintillation properties of Ce³⁺ doped yttrium aluminum perovskite (YAP:Ce) crystals was investigated. Crystals with slight yttrium excess (Y₁_·₀₀₄AlO₃:Ce), yttrium deficiency (Y₀_·₉₉₄AlO₃:Ce), and stoichiometric composition (YAlO₃:Ce) were synthesized using the micro-pulling down method. Structural characterization confirmed crystallization in the pure orthorhombic Pnma space group for all compositions. Optical absorption spectroscopy revealed an extensive background in the nonstoichiometric crystals due to the increased degree of light scattering centers associated with the defects. The photoluminescence excitation and emission spectra of Ce³⁺ ions were unaffected by nonstoichiometry. However, the scintillation decay kinetics and light yield exhibited marked improvements in the Y_1±xAlO₃:Ce (x≠0) crystals. The light yield increased by 22 % and 15 % and the slower component of the decay accelerated from 171 ns to 106 and 131 ns compared to the stoichiometric crystal. Thermoluminescence glow curves revealed that nonstoichiometry significantly altered the concentrations of antisite defects and oxygen vacancies. The EPR spectroscopy investigations revealed a correlation between the Ce³⁺ ions concentration and the degree of nonstoichiometry. Strategic engineering of nonstoichiometry in Y_1±xAlO₃:Ce (x≠0) scintillators may have provided an effective approach to optimizing scintillation performance.

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通过非化学计量工程实现掺杂 Ce3+ 的 Y1±xAlO3 (x≠0) 单晶包晶闪烁体的进步

研究了非化学计量工程对掺杂 Ce3+ 的钇铝包晶石（YAP:Ce）晶体闪烁特性的影响。采用微拉法合成了轻微钇过量（Y1-004AlO3:Ce）、钇缺乏（Y0-994AlO3:Ce）和化学计量成分（YAlO3:Ce）的晶体。结构表征证实，所有成分都在纯正正方形 Pnma 空间群中结晶。光学吸收光谱显示，由于与缺陷相关的光散射中心程度增加，非全度晶体中存在大量背景。Ce3+ 离子的光致发光激发光谱和发射光谱不受非化学计量的影响。然而，Y1±xAlO3:Ce（x≠0）晶体的闪烁衰减动力学和光产率有了明显改善。与化学计量晶体相比，光产率分别增加了 22% 和 15%，衰减的慢速部分从 171 ns 加速到 106 ns 和 131 ns。热释光辉光曲线显示，非全度性显著改变了反斜长石缺陷和氧空位的浓度。EPR 光谱研究表明，Ce3+ 离子浓度与非均匀度之间存在相关性。对 Y1±xAlO3:Ce (x≠0) 闪烁器中的非全度进行战略性设计，可能是优化闪烁性能的有效方法。

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