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

Meng Meng; Qi Qiang; He Chong-Jun; Ding Dong-Zhou; Zhao Shu-Wen; Shi Jun-Jie; Ren Guo-Hao

doi:10.7498/aps.70.20201697

Abstract

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 Gd_Al/Ga antisite-defect at 380 nm. The emission intensity of Gd_Al/Ga antisite-defect in the lack of (Al,Ga) component is higher than that in the excess (Al,Ga) component. The inclusions and Gd_Al/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 Gd_Al/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 Gd_Al/Ga antisite-defect and crystal composition, and provide a theoretical basis for restraining the defects and improving the crystal properties.

Keywords:

Authors and contacts

1.
Key Laboratory of Space Photoelectric Detection and Perception, Ministry of Industry and Information Technology, College of Astronautics, Nanjing University of Aeronautics and Astronautics, Nanjing 210016, China
2.
Shanghai Institute of Ceramics, Chinese Academy of Sciences, Shanghai 201899, China
3.
Haixi Institute of Innovation, Chinese Academy of Sciences, Fuzhou 350002, China
4.
School of Materials Science and Engineering, University of Shanghai for Science and Technology, Shanghai 200093, China
5.
State Key Laboratory of Crystal Materials, Shandong University, Jinan 250100, China

Corresponding author: He Chong-Jun, hechongjun@nuaa.edu.cn ; Ding Dong-Zhou, dongzhou_ding@mail.sic.ac.cn ;

Funds: Project supported by the National Natural Science Foundation of China (Grant No. 61675095), the Key Technical Talents of the Chinese Academy of Sciences, China (Grant No. Y74YQ3130G), the Independent Deployment Project of Hercynian Research Institute of Chinese Academy of Sciences, China (Grant No. FJCXY18040202), the Open Project Funds for the Key Laboratory of Space Photoelectric Detection and Perception (Nanjing University of Aeronautics and Astronautics), Ministry of Industry and Information Technology, China (Grant No. NJ2020021-2), and the Fundamental Research Funds for the Central Universities of Ministry of Education of China (Grant No. NJ2020021)

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References

[1]	何伟, 张约品, 王金浩, 王实现, 夏海平 2011 物理学报 60 042901 Google Scholar He W, Zhang Y P, Wang J H, Wang S X, Xia H P 2011 Acta Phys. Sin. 60 042901 Google Scholar
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[3]	Sakthong O, Chewpraditkul W, Wanarak C, Kamada K, Yoshikawa A, Prusa P, Nikl M 2014 Nucl. Instrum. Methosds Phys. Res. A 751 1 Google Scholar
[4]	Tamagawa Y, Inukai Y, Ogawa I, Kobayashi M 2015 Nucl. Instrum. Methods Phys. Res. A 795 192 Google Scholar
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[21]	杨斌, 张约品, 徐波, 来飞, 夏海平, 赵天池 2012 物理学报 61 192901 Google Scholar Yang B, Zhang Y P, Xu B, Lai F, Xia H P, Zhao T C 2012 Acta Phys. Sin. 61 192901 Google Scholar
[22]	Zorenko Y 2005 Phys. Status Solidi C 26 375 Google Scholar

Cited By

图 1 GAGG:Ce晶体及样品照片

Figure 1. Photos of GAGG:Ce crystal and samples.

DownLoad: Full-Size Img PowerPoint

图 2 GAGG:Ce样品粉末XRD图谱

Figure 2. XRD patterns of GAGG:Ce crystal.

DownLoad: Full-Size Img PowerPoint

图 3 GAGG:Ce晶体的能级结构图(a)与透过谱(b)

Figure 3. Energy diagram (a) and transmittance (b) of GAGG:Ce crystal sample.

DownLoad: Full-Size Img PowerPoint

图 4 GAGG:Ce晶体微区形貌分析　(a) 片状包裹体; (b) 黑白相间状包裹体

Figure 4. Micro-region morphology analysis of GAGG:Ce crystal: (a) Lamellar inclusions; (b) black and white interphase inclusions.

DownLoad: Full-Size Img PowerPoint

图 5 GAGG:Ce晶体的X射线激发发射谱(a)和积分强度(b)

Figure 5. X-ray excited spectra (a) and integrated intensity (b) of GAGG:Ce crystal.

DownLoad: Full-Size Img PowerPoint

图 6 室温下GAGG:Ce样品在¹³⁷Cs源激发下的多道能谱(HV, 高压)

Figure 6. Multi-channel energy spectra of GAGG:Ce crystal excited by ¹³⁷Cs (HV, high voltage)

DownLoad: Full-Size Img PowerPoint

图 7 不同基质成分的GAGG:Ce晶体能级示意图

Figure 7. Schematic energy level diagrams of GAGG:Ce crystal with different matrix components.

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图 8 GAGG:Ce晶体归一化后的光产额与成形时间相关性. 以0.75 μs为标准, 实线为模型拟合曲线

Figure 8. Light yield dependence on amplifier shaping time normalized at 0.75 μs for GAGG:Ce crystal, where solid lines are the fitting curve.

DownLoad: Full-Size Img PowerPoint

图 9 GAGG:Ce晶体的闪烁衰减时间

Figure 9. Scintillation decay curve of GAGG:Ce crystal

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表 1 GAGG:Ce晶体的EDS成分分析

Table 1. Composition analysis data by EDS of GAGG:Ce crystal.

Sample	Gd	Al	Ga	Al + Ga
Sample	ion ratio
1	3.034	2.274	2.692	4.966
2	2.985	2.213	2.802	5.015
Theoretical value	3	2.3	2.7	5

DownLoad: CSV

表 2 GAGG:Ce晶体的晶胞参数

Table 2. Lattice parameters of GAGG:Ce crystal at different positions.

Sample	1	2
Diffractive angle (2θ)/(°)	32.8	32.73
Lattice parameters/nm	12.2492	12.2516

DownLoad: CSV

表 3 GAGG:Ce晶体的EDS能谱微区成分分析数据

Table 3. Micro-region composition analysis data by EDS of GAGG:Ce crystal.

取样点	Gd	Ce	Al	Ga	Al + Ga	O	(Gd + Ce)∶(Al + Ga)∶O
取样点	Atomic percentage						离子数之比
1	17.61	—	10.33	12.06	22.39	60	3.5∶4.5∶12
2	14.97	—	11.11	13.92	25.03	60	3∶5∶12
3	3.71	20.57	4.45	11.26	15.71	60	4.9∶3.1∶12
4	1.19	—	17.9	20.91	38.81	60	0.06∶2∶3
5	15.06	—	10.63	14.31	24.94	60	3∶5∶12

DownLoad: CSV

[1]	何伟, 张约品, 王金浩, 王实现, 夏海平 2011 物理学报 60 042901 Google Scholar He W, Zhang Y P, Wang J H, Wang S X, Xia H P 2011 Acta Phys. Sin. 60 042901 Google Scholar
[2]	孟猛, 祁强, 丁栋舟, 赫崇君, 施俊杰, 任国浩 2019 人工晶体学报 48 8 Google Scholar Meng M, Qi Q, Ding D Z, He C J, Shi J J, Ren G H 2019 J. Synth. Cryst. 48 8 Google Scholar
[3]	Sakthong O, Chewpraditkul W, Wanarak C, Kamada K, Yoshikawa A, Prusa P, Nikl M 2014 Nucl. Instrum. Methosds Phys. Res. A 751 1 Google Scholar
[4]	Tamagawa Y, Inukai Y, Ogawa I, Kobayashi M 2015 Nucl. Instrum. Methods Phys. Res. A 795 192 Google Scholar
[5]	Kochurikhin V, Kamada K, Kim J, Ivanov M, Yoshikawa A 2020 J. Cryst. Growth 531 1 Google Scholar
[6]	冯大建, 丁雨憧, 刘军, 李和新, 付昌禄, 胡少勤 2016 压电与声光 38 430 Feng D J, Ding Y C, Liu J, Li H X, Fu C L, Hu S Q 2016 Piezoelectrics Acoustooptics 38 430
[7]	Kamada K, Takayuki A, Yanagida T, Endo T, Tsutumi K, Usuki Y, Nikl M, Fujimoto Y, Fukabori A, Yoshikawa A 2012 J. Cryst. Growth 352 88 Google Scholar
[8]	Wang C, Wu Y T, Ding D Z, Li H Y, Chen X F, Shi J, Ren G H 2016 Nucl. Instrum. Methods Phys. Res. A 820 8 Google Scholar
[9]	Chewpraditkul W, Panek D, Bruza P, Chewpraditkul W, Wanarak C, Pattanaboonmee N, Babin V, Bartosiewicz K, Kamada K, Yoshikawa A, Nikl M 2014 J. Appl. Phys. 116 083505 Google Scholar
[10]	Kitaura M, Watanabe S, Kamada K, Kim J K, Yoshino M, Kurosawa S, Yagihashi T, Ohnishi A, Hara K 2018 Appl. Phys. Lett. 113 041906 Google Scholar
[11]	丁栋舟, 李焕英, 秦来顺, 卢胜, 潘尚可, 任国浩 2010 无机材料学报 25 1021 Google Scholar Ding D Z, Li H Y, Qin L S, Lu S, Pan S K, Ren G H 2010 J. Inorg. Mater. 25 1021 Google Scholar
[12]	孟猛, 祁强, 丁栋舟, 赫崇君, 赵书文, 万博, 陈露, 施俊杰, 任国浩 2020 无机材料学报 Google Scholar Meng M, Qi Q, Ding D Z, He C J, Zhao S W, Wan B, Chen L, Shi J J, Ren G H 2020 J. Inorg. Mater.Google Scholar
[13]	鲁万成, 张庆礼, 罗建乔, 丁守军, 窦仁勤, 彭方, 张会丽, 王小飞, 孙贵花, 孙敦陆 2017 物理学报 66 154204 Google Scholar Lu W C, Zhang Q L, Luo J Q, Ding S J, Dou R Q, Peng F, Zhang H L, Wang X F, Sun G H, Sun D L 2017 Acta Phys. Sin. 66 154204 Google Scholar
[14]	Kurosawa S, Shoji Y, Yokota Y, Kamada K, Chani V, Yoshikawa A 2014 J. Cryst. Growth 393 134 Google Scholar
[15]	Etiennette A, Ramunas A, Andrei F, Georgy D, Larisa G, Vidmantas G, Merry K, Marco L, Charles M, Saulius L, Gintautas T, Augustas V, Aleksejs Z, Mikhail K 2018 Phys. Status Solidi A 215 1700798 Google Scholar
[16]	Mares J A, Nikl M, Beitlerova A, Solovieva N, Ambrosio C, Blazek K, Maly P, Nejezchle K, Fabeni P, Pazzi P 2005 Nucl. Instrum. Methods Phys. Res. A 537 271 Google Scholar
[17]	Stanek C R, McClellana C J, Levyb M R, Milanese C, Grimes R W 2007 Nucl. Instrum. Methods Phys. Res. A 579 27 Google Scholar
[18]	杨新波, 石云, 李红军, 毕群玉, 苏良碧, 刘茜, 潘裕柏, 徐军 2009 物理学报 58 8050 Google Scholar Yang X B, Shi Y, Li H J, Bi Q Y, Su L B, Liu Q, Pan Y B, Xu J 2009 Acta Phys. Sin. 58 8050 Google Scholar
[19]	Yoshino M, Kamada K, Shoji Y, Yamaji A, Kurosawa S, Kurosawa Y, Ohashi Y, Yoshikawa A, Chani V 2017 J. Cryst. Growth 468 420 Google Scholar
[20]	Kamada K, Kurosawa S, Prusa P, Nikl M, Kochurikhin V, Endo T, Tsutumi K, Sato H, Yokota K, Y, Sugiyama K, Yoshikawa A 2014 Opt. Mater. 36 1942 Google Scholar
[21]	杨斌, 张约品, 徐波, 来飞, 夏海平, 赵天池 2012 物理学报 61 192901 Google Scholar Yang B, Zhang Y P, Xu B, Lai F, Xia H P, Zhao T C 2012 Acta Phys. Sin. 61 192901 Google Scholar
[22]	Zorenko Y 2005 Phys. Status Solidi C 26 375 Google Scholar

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

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Authors and contacts

Corresponding author: He Chong-Jun, hechongjun@nuaa.edu.cn ; Ding Dong-Zhou, dongzhou_ding@mail.sic.ac.cn ;

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