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中国物理学会期刊

Gd3(Al,Ga)5O12:Ce闪烁晶体缺陷对其发光性能的影响

CSTR: 32037.14.aps.70.20201697

Influence of defects on luminescence properties of Gd3(Al,Ga)5O12:Ce scintillation crystals

CSTR: 32037.14.aps.70.20201697
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  • 新型闪烁晶体Gd3(Al,Ga)5O12:Ce (GAGG:Ce)在制备过程中易出现包裹体及反格位缺陷等问题, 严重影响晶体的性能. 为了抑制这些缺陷以得到大尺寸高质量的GAGG:Ce晶体, 本文以Gd3(Al,Ga)5O12为基质、Ce3+为掺杂离子, 采用提拉法生长得到了GAGG:Ce晶体, 并对不同晶体部位的物相结构、微区成分、透光性质、发光及时间性能进行了测试和对比分析. 结果表明, GAGG:Ce晶体的透过谱中存在340和440 nm两处Ce3+特征吸收带, 且位于550 nm处的直线透过率为82%. 晶体尾部因杂相包裹体等宏观缺陷的影响, 导致其透过率下降至70%左右. 微区成分分析进一步表明GAGG:Ce晶体中存在三种类型的包裹体, 分别为富Gd相、富Ce相及(Al,Ga)2O3相. GAGG:Ce晶体的X射线激发发射谱中在550 nm附近存在Ce3+宽发射带, 且380 nm处还存在GdAl/Ga反格位缺陷引起的发射. 晶体中存在的杂相包裹体及GdAl/Ga反格位缺陷等因素导致Ce3+在GAGG基质的发光强度下降12.5%; GdAl/Ga反格位离子与近邻Ce的隧穿效应使得GAGG:Ce晶体的衰减时间由117.7 ns延长至121.9 ns, 且慢分量比例由16%增加至17.2%.

     

    There are many problems during the preparation of the scintillation crystal Gd3(Al,Ga)5O12:Ce (abbreviated as GAGG:Ce), such as inclusions and antisite-defect. In order to inhibit these defects and obtain large-size and high-quality GAGG:Ce crystal, this study uses Gd3(Al,Ga)5O12 as the matrix and Ce3+ as the doping ions to grow the GAGG:Ce crystal by the Czochralski method. The phase structure, micro-region composition, optical and scintillation properties of GAGG:Ce are tested and compared. It is found that tipical Ce3+ absorption bands are at 340 nm and 440 nm, and the linear transmittance at 550 nm is 82%. The transmittance of the crystal tail drops to about 70% due to the macroscopic defects such as inclusions. The micro-region composition analysis shows that the three types of inclusions in GAGG:Ce crystal are Gd-rich phase, Ce-rich phase, and (Al,Ga)2O3 phase. The Ce3+ ion emission wavelength of GAGG:Ce crystal is about 550 nm excited by the X-ray, and there is also an emission wavelength caused by the GdAl/Ga antisite-defect at 380 nm. The emission intensity of GdAl/Ga antisite-defect in the lack of (Al,Ga) component is higher than that in the excess (Al,Ga) component. The inclusions and GdAl/Ga antisite-defect make the luminous efficiency of GAGG:Ce crystal decrease by 12.5% and the corresponding light yield decreases from 58500 to 52000 photon/MeV. The tunneling effect between GdAl/Ga antisite-defect ions and neighboring Ce3+ ions makes the decay time of the GAGG:Ce crystal extend from 117.7 to 121.9 ns, and the ratio of slow component increases from 16% to 17.2%. The migration of energy along the Gd3+ sublattice makes the rise time of the GAGG:Ce crystal extend from 8.6 to 10.7 ns. The above conclusions further deepen the understanding of the source of inclusions and the relationship between the GdAl/Ga antisite-defect and crystal composition, and provide a theoretical basis for restraining the defects and improving the crystal properties.

     

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