首页> 外文期刊>The journal of physical chemistry, A. Molecules, spectroscopy, kinetics, environment, & general theory >Luminescence and energy transfer in Lu _3Al _5O _(12) scintillators co-doped with Ce ~(3+) and Tb ~(3+)
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Luminescence and energy transfer in Lu _3Al _5O _(12) scintillators co-doped with Ce ~(3+) and Tb ~(3+)

机译:Ce〜(3+)和Tb〜(3+)共掺杂的Lu _3Al _5O _(12)闪烁体的发光和能量转移

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摘要

Lu _3Al _5O _(12) (LuAG) doped with Ce ~(3+) is a promising scintillator material with a high density and a fast response time. The light output under X-ray or γ-ray excitation is, however, well below the theoretical limit. In this paper the influence of codoping with Tb ~(3+) is investigated with the aim to increase the light output. High resolution spectra of singly doped LuAG (with Ce ~(3+) or Tb ~(3+)) are reported and provide insight into the energy level structure of the two ions in LuAG. For Ce ~(3+) zerophonon lines and vibronic structure are observed for the two lowest energy 5d bands and the Stokes' shift (2 350 cm ~(-1)) and HuangRhys coupling parameter (S = 9) have been determined. Tb ~(3+) 4f-5d transitions to the high spin (HS) and low spin (LS) states are observed (including a zerophonon line and vibrational structure for the high spin state). The HS-LS splitting of 5400 cm ~(-1) is smaller than usually observed and is explained by a reduction of the 5d-4f exchange coupling parameter J by covalency. Upon replacing the smaller Lu ~(3+) ion with the larger Tb ~(3+) ion, the crystal field splitting for the lowest 5d states increases, causing the lowest 5d state to shift below the 5D4 state of Tb ~(3+) and allowing for efficient energy transfer from Tb ~(3+) to Ce ~(3+) down to the lowest temperatures. Luminescence decay measurements confirm efficient energy transfer from Tb ~(3+) to Ce ~(3+) and provide a qualitative understanding of the energy transfer process. Codoping with Tb ~(3+) does not result in the desired increase in light output, and an explanation based on electron trapping in defects is discussed.
机译:掺杂有Ce〜(3+)的Lu _3Al _5O _(12)(LuAG)是一种有前途的闪烁体材料,具有高密度和快速响应时间。但是,在X射线或γ射线激发下的光输出远低于理论极限。本文研究了共掺杂对Tb〜(3+)的影响,旨在增加光输出。报告了单掺杂LuAG(具有Ce〜(3+)或Tb〜(3+))的高分辨率光谱,并提供了对LuAG中两个离子能级结构的了解。对于Ce〜(3+)零声子线和振动子结构,观察到两个最低能量的5d谱带,并确定了斯托克斯位移(2 350 cm〜(-1))和HuangRhys耦合参数(S = 9)。观察到Tb〜(3+)4f-5d转变为高自旋(HS)和低自旋(LS)态(包括零声子线和高自旋态的振动结构)。 5400 cm〜(-1)的HS-LS分裂比通常观察到的要小,并且可以通过5d-4f交换耦合参数J的共价降低来解释。在用较大的Tb〜(3+)离子替换较小的Lu〜(3+)离子后,对于最低5d态的晶体分裂增加,导致最低5d态移动到Tb〜(3+)的5D4态以下。 )并允许从Tb〜(3+)到Ce〜(3+)的能量有效转移至最低温度。发光衰减测量结果证实了从Tb〜(3+)到Ce〜(3+)的有效能量转移,并提供了对能量转移过程的定性理解。与Tb〜(3+)共掺杂不会导致所需的光输出增加,并且将讨论基于缺陷中电子陷阱的解释。

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