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阳离子对KRE(PO)₄:Ce/Pr(RE = La、Gd和Y)磷光体用于X射线检测的光致发光和X射线辐射发光的影响

Cationic Effects on Photo- and X-ray Radioluminescence of KRE(PO):Ce/Pr (RE = La, Gd, and Y) Phosphors toward X-ray Detection.

作者信息

Ou Yiyi, Zhou Weijie, Dorenbos Pieter, Liang Hongbin

机构信息

MOE Key Laboratory of Bioinorganic and Synthetic Chemistry, KLGHEI of Environment and Energy Chemistry, School of Chemistry, Sun Yat-sen University, Guangzhou 510006, China.

Department of Radiation Science and Technology, Faculty of Applied Sciences, Delft University of Technology, Mekelweg 15, 2629 JB Delft, The Netherlands.

出版信息

Inorg Chem. 2023 Apr 17;62(15):6181-6188. doi: 10.1021/acs.inorgchem.3c00566. Epub 2023 Apr 5.

Abstract

Cationic tuning for lanthanide (Ce/Pr)-activated inorganic phosphors with stable, efficient, and fast-decay 5d-4f emissions has emerged as an important strategy toward the continuing pursuit of superior scintillators. The in-depth understanding of the cationic effects on photo- and radioluminescence of lanthanides Ce and Pr centers is requisite for the rational cationic tuning. Here, we perform a systematic study on the structure and photo- and X-ray radioluminescence properties of KRE(PO):Ce/Pr (RE = La, Gd, and Y) phosphors to elucidate the underlying cationic effects on their 4f-5d luminescence. By using the Rietveld refinements, low-temperature synchrotron-radiation vacuum ultraviolet-ultraviolet spectra, vibronic coupling analyses, and vacuum-referred binding energy schemes, the origins of lattice parameter evolutions, 5d excitation energies, 5d emission energies, and Stokes shifts as well as good emission thermal stabilities of KRE(PO):Ce systems are revealed. In addition, the correlations of Pr luminescence to Ce in the same sites are also discussed. Finally, the X-ray excited luminescence manifests that the KGd(PO):1%Ce sample possesses a light yield of ∼10,217 photons/MeV, indicating its potentiality toward X-ray detection application. These results deepen the understanding of cationic effects on Ce and Pr 4f-5d luminescence and inspire the inorganic scintillator development.

摘要

对于具有稳定、高效且快速衰减的5d-4f发射的镧系(Ce/Pr)激活无机磷光体而言,阳离子调控已成为持续追求卓越闪烁体的一项重要策略。深入了解阳离子对镧系元素Ce和Pr中心的光致发光和辐射发光的影响,对于合理的阳离子调控是必不可少的。在此,我们对KRE(PO):Ce/Pr(RE = La、Gd和Y)磷光体的结构、光致发光和X射线辐射发光特性进行了系统研究,以阐明阳离子对其4f-5d发光的潜在影响。通过使用Rietveld精修、低温同步辐射真空紫外-紫外光谱、振动耦合分析以及真空参考结合能方案,揭示了KRE(PO):Ce体系中晶格参数演变、5d激发能、5d发射能、斯托克斯位移以及良好发射热稳定性的起源。此外,还讨论了同一位置上Pr发光与Ce的相关性。最后,X射线激发发光表明KGd(PO):1%Ce样品的光产额约为10217光子/MeV,表明其在X射线检测应用方面的潜力。这些结果加深了对阳离子对Ce和Pr 4f-5d发光影响的理解,并推动了无机闪烁体的发展。

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