Twisted Growth, Component Segregation and Characteristics of Gd3(Al,Ga)5O12:Ce Scintillation Crystal

doi:10.15541/jim20200268

Abstract

Abstract:

There are many problems such as polycrystal twisted growth and component segregation during the preparation of the new scintillation crystal Gd₃(Al,Ga)₅O₁₂:Ce (abbreviated as GAGG:Ce) by the Czochralski method. In order to solve these problems to obtain large-size and high-quality GAGG:Ce crystals, with a combination of melt characteristics, formation mechanism of twisted growth, component segregation, spectral characteristics and scintillation performance of GAGG:Ce crystals were studied. A complete GAGG:Ce crystal with size of ?50 mm× 120 mm was successfully grown by adjusting the temperature field and inhibiting the volatilization of the components. The results show that light output of the GAGG:Ce crystal sample (10 mm×10 mm×2 mm) is 58000 ph./MeV, while energy resolution is 6.4%@662 keV with transmittance at 550 nm of 82%, decay time of 126 ns (83%), and the slow component is 469 ns (17%). The peak position of emission wavelength of the crystal is about 550 nm, which matches well with the silicon photomultiplier. Meanwhile, the emission weighted longitudinal transmittance is as high as 79.8%. GAGG:Ce crystal has an excellent combination of high light output and energy resolution, and all of these properties show that GAGG:Ce crystal is a promising scintillator for neutron and gamma detection applications.

Key words: polycrystal twisted growth, temperature gradient, component segregation, decay time

CLC Number:

O734

MENG Meng, QI Qiang, DING Dongzhou, HE Chongjun, ZHAO Shuwen, WAN Bo, CHEN Lu, SHI Junjie, REN Guohao. Twisted Growth, Component Segregation and Characteristics of Gd₃(Al,Ga)₅O₁₂:Ce Scintillation Crystal[J]. Journal of Inorganic Materials, 2021, 36(2): 188-196.

Figures/Tables 17

Fig. 1 Photo of polycrystal twisted growth GAGG:Ce crystal

Fig. 2 Photo and XRD pattern of volatiles during crystal growth of GAGG:Ce: (a) volatiles photo; (b) XRD pattern

Fig. 3 Gd2O3-Ga2O3 phase diagram[11] (a) Phase region of stable phase; (b) Phase region of metastable phase

Table 1 Component analysis data by Inductively Coupled Plasma Optical Emission Spectrum (ICP-OES) of polycrystal twisted growth samples

Sample	n_Gd : n_Al : n_Ga
Melt	3.0 : 2.3 : 2.7
Twisted growth crystal	3.00 : 3.57 : 0.83

Fig. 4 XRD patterns of polycrystal twisted growth crystal powder

Fig. 5 Random protrusions, indentations and iridium attachments of GAGG:Ce crystal

Fig. 6 Photo of GAGG:Ce Crystal with partial component

Table 2 Component analysis data by Inductively Coupled Plasma Optical Emission Spectrum (ICP-OES) of crystal head and tail samples

Sample	n_Gd : n_A : n_Ga
Melt	3.0 : 2.3 : 2.7
Crystal head	3.00 : 3.56 : 1.57
Crystal tail	3.0 : 2.3 : 2.7

Fig. 7 XRD patterns of crystal head and tail powder

Table 3 Component analysis data by Electronic Differential System (EDS) of GAGG:Ce crystal

Spectrum	Mole fraction/mol%				Ratio of ions
Spectrum	Gd	Ce	Al+Ga	O	Gd:(Al+Ga):O
1 (inclusion)	20.61	-	19.39	60	1 : 1 : 3
2 (matrix)	14.97	-	25.03	60	3 : 5 : 12

Fig. 8 SEM image of GAGG:Ce crystal

Fig. 9 X-ray excited spectra of partial crystal and ceramics (a) Head and tail of partial crystal; (b) GdAl0.5Ga0.5O3:Ce (GAGP:Ce), Gd3Al2.5Ga2.5O3:Ce (GAGG:Ce), and Gd4Al2O9:Ce (GAM:Ce)

Fig. 10 Photo of GAGG:1%Ce crystal grown by Czochralski method

Fig. 11 Transmission and X-ray excited spectra of GAGG:1% crystal at room temperature Black solid line representing the transmittance; Red solid line representing the X-ray excited spectra; Blue solid dots representing the theoretical limit of transmittance calculated from the measured refractive indices N

Table 4 Refractive index and theoretical transmittance of GAGG:1%Ce crystal

Parameter	λ/nm
Parameter	400	475	520	575	625	700
n	1.951	1.919	1.91	1.904	1.9	1.898
T/%	81.17	81.97	82.18	82.34	82.43	82.48

Fig. 12 Multi-channel energy spectra of GAGG:1%Ce crystal excited by 137Cs

Fig. 13 GAGG:1%Ce crystal time behavior (a) Light output curve at different time Gates and its fitted line; (b) Scintillation decay curve and its fitted line

References 22

[1]	MENG MENG, QI QIANG, DING DONG-ZHOU, et al. Research progress on novel scintillation crystal Gd₃(Al,Ga)₅O₁₂:Ce³⁺. Journal of Synthetic Crystals, 2019,48(8):1386-1394.
[2]	VAN EIJK C. Inorganic Scintillators in Positron Emission Tomography. Radiation Detectors for Medical Applications. Netherland: Springer Netherlands, 2006: 259-274.
[3]	KAMADA K, TAKAYUKI A, YANAGIDA T, et al. 2 inch diameter single crystal growth and scintillation properties of Ce:Gd₃Al₂Ga₃O₁₂. Journal of Crystal Growth, 2012,352(1):88-90.
[4]	TAMAGAWA Y, INUKAI Y, OGAWA I, et al. Alpha-gamma pulse-shape discrimination in Gd₃Al₂Ga₃O₁₂:Ce³+ crystal scintillator using shape indicator. Nuclear Instruments and Methods in Physics Research, 2015,795(21):192-195.
[5]	KOCHURIKHIN V, KAMADA K, IVANOV M, et al. Czochralski growth of 4-inch diameter Ce:Gd₃Al₂Ga₃O₁₂single crystals for scintillator applications. Journal of Crystal Growth, 2020,531:1.
[6]	FENG DA-JIAN. Study on the growth and scintillation properties of Ce:GAGG crystal. Piezoelectrics and Acoustooptics, 2016,38(3):430-432.
[7]	WANG CHAO, WU YUN-TAO, DING DONG-ZHOU, et al. Optical and scintillation properties of ce-doped (Gd₂Y₁)Ga_2.7Al_2.3O₁₂, single crystal grown by Czochralski method. Nuclear Instruments and Methods in Physics Research A, 2016,820:8-13.
[8]	YUAN HANG, CHEN YU-XIAO, WANG YING-JIE, et al. Inorganic scintillator gadolinium gallium aluminum garnet (GAGG)’s performance research and application. Modern Industrial Economy and Informationization, 2018,8(11):24-26.
[9]	SHISHIDO T, OKAMURA K, YAJIMA S. Gd₃Al₅O₁₂ phase obtained by crystallization of amorphous Gd₂O₃·5/3Al₂O₃. J. Am. Ceram. Soc., 1978,61(7/8):37-375.
[10]	ASADIAN M, HAJIESMAEILBAIGI F, MIRZAEI N, et al. Composition and dissociation processes analysis in crystal growth of Nd:GGG by the Czochralski method. Journal of Crystal Growth, 2010,312(9):1645-1650.
[11]	DIGIUSEPPE A, SOLED L, WENNER M, et al. Phase diagram relationships of the garnet-perovskite transformation in the Gd₂O₃-Ga₂O₃ and Sm₂O₃-Ga₂O₃ systems. Progress in Crystal Growth and Characterization of Materials, 1980,49(4):746-748.
[12]	DING DONG-ZHOU, LI HUAN-YING, QIN LAI-SHUN, et al. Research on the defects in Lu_xY₁-_xAlO₃:Ce crystals. Journal of Inorganic Materials, 2010,25(10):1021-1024.
[13]	KAMADA K, NIKL M, KUROSAWA S, et al. Alkali earth co-doping effects on luminescence and scintillation properties of Ce-doped Gd₃Al₂Ga₃O₁₂ scintillator. Optical Materials, 2015,41(13):63-66.
[14]	ZHANG YE, CHEN XIAN-QIANG, QIN HAI-MING, et al. Fabrication of Ce-doped Gd₃(Al,Ga)₅O₁₂ powders using Co-precipitation Method. Journal of Inorganic Materials, 2016,31(10):1151-1156.
[15]	KUCERA M, HANUS M, ONDERISINOVA Z, et al. Energy transfer and scintillation properties of Ce³⁺ doped (Lu,Y,Gd)₃(Al,Ga)₅O₁₂multicomponent garnets. IEEE Transactions on Nuclear Science, 2014,61(1):282-289.
[16]	VERWEIJ J, COHEN M, BOUTTET D, et al. Luminescence properties of GdAlO₃:Ce powders. Chemical Physics Letters, 1995,239(1/2/3):51-55.
[17]	SINHA A, SHARMA B, GOPALAN P, et al. Study on phase evolution of GdAl₁-_xGa_xO₃ system. Journal of Alloys and Compounds, 2009,492(2010):325-330.
[18]	ETIENNETTE A, RAMUNAS A, ANDREI F, et al. Excitation transfer engineering in Ce-doped oxide crystalline scintillators by codoping with alkali-earth ions. Physica Status Solidi A, 2018,215(7):1700798.
[19]	KOZLOVA N S, BUSANOV O A, ZABELINA E V, et al. Optical properties and refractive indices of Gd₃Al₂Ga₃O₁₂:Ce³+ crystals. Crystal Lography Reports, 2016,61(3):474-478.
[20]	ZELMON D E, SMALL D L, PAGE R. Refractive-index measurements of undoped yttrium aluminum garnet from 0.4- 5.0 μm. Applied Optics, 1998,37(21):4933-4935. URL PMID
[21]	ZHANG GUO-QING, YANG FAN, WU YUN-TAO, et al. Influence of F/Cl ratio on the crystal growth and luminescence properties of PbFCl crystals. Journal of Inorganic Materials, 2014,29(2):162-166.
[22]	YOSHIHO M, KAMADA K, SHOJI Y, et al. Effect of Mg co-doping on scintillation properties of Ce:Gd₃(Ga,Al)₅O₁₂single crystals with various Ga/Al ratios. Journal of Crystal Growth, 2017,468:420-423.

Twisted Growth, Component Segregation and Characteristics of Gd₃(Al,Ga)₅O₁₂:Ce Scintillation Crystal

RichHTML

PDF (PC)

Knowledge

Abstract

Cite this article

share this article

Figures/Tables 17

References 22

Related Articles 13

Recommended Articles

Metrics

Comments

[1]	HAO Yongxin, QIN Juan, SUN Jun, YANG Jinfeng, LI Qinglian, HUANG Guijun, XU Jingjun. Impact of Crucible Bottom Shape on the Growth of Congruent Lithium Niobate Crystals by Czochralski Method [J]. Journal of Inorganic Materials, 2024, 39(10): 1167-1174.
[2]	LI Mingqing, WANG Linwei, DING Dongzhou, FENG He. Mechanism of Mg-codoping in Improving the Time Performance of Gd₃(Al,Ga)₅O₁₂:Ce Scintillator [J]. Journal of Inorganic Materials, 2022, 37(10): 1123-1128.
[3]	REN Guo-Hao, SONG Zhao-Hui, ZHANG Zi-Chuan, ZHANG Kan, YANG Fan, LI Huan-Ying, CHEN Xiao-Feng. Luminescence and Decay Time Properties of Pure CsI Crystals [J]. Journal of Inorganic Materials, 2017, 32(2): 169-174.
[4]	LI Feng-Rui, GU Mu, HE Hui, CHANG Li-Hua, WEN Wei-Feng, LI Ze-Ren, CHEN Liang, LIU Jin-Liang, OUYANG Xiao-Ping, LIU Xiao-Lin, LIU Bo, HUANG Shi-Ming,NI Chen. Fluorescent Decay Time and Energy Response of γ-CuI Crystal [J]. Journal of Inorganic Materials, 2017, 32(2): 163-168.
[5]	ZHANG Guo-Qing, YANG Fan, WU Yun-Tao, SUN Dan-Dan, SHANG Shan-Shan, REN Guo-Hao. Influence of F/Cl Ratio on the Crystal Growth and Luminescence Properties of PbFCl Crystals [J]. Journal of Inorganic Materials, 2014, 29(2): 162-166.
[6]	SUN Dan-Dan, PAN Shang-Ke, REN Guo-Hao, WU Yun-Tao, SHANG Shan-Shan, ZHANG Guo-Qing. Luminescence Properties of High Y³⁺-doped Ce:Li₆Lu(BO₃)₃ Scintillators [J]. Journal of Inorganic Materials, 2013, 28(9): 987-991.
[7]	HU Ke-Yan, XU Jun, TANG Hui-Li, LI Hong-Jun, ZOU Yu-Qi, YANG Qiu-Hong. Study on Methods to Strenthen and Toughen Sapphire Crystal by Carbon Doped Grown by Temperature Gradient Technique (TGT) [J]. Journal of Inorganic Materials, 2013, 28(3): 307-311.
[8]	ZHANG Kai,LIU He-Zhou,WU Ya-Ting,HU Wen-Bin. Temperature Dependence of Luminescence and Decay Time of YAG:Ce Nanophosphor [J]. Journal of Inorganic Materials, 2008, 23(5): 1045-1048.
[9]	AN Li-Qiong,ZHANG Jian,LIU Min,WANG Shi-Wei. Spectroscopic Study of Lu₂O₃:Yb³⁺, Ho³⁺Nanopowders [J]. Journal of Inorganic Materials, 2008, 23(2): 383-386.
[10]	ZOU Ji-Zhao,ZENG Xie-Rong,XIONG Xin-Bo,LI Xiao-Hua,TANG Han-Ling,LI Long. Microwave Heating Effect and Mechanism for Carbon Fiber Preforms [J]. Journal of Inorganic Materials, 2007, 22(6): 1165-1168.
[11]	CHEN Jun-Feng,LI Yun,SONG Gui-Lan,YAO Dong-Min,YUAN Lan-Ying,QI Xue-Jun,WANG Shao-Hua. Temperature Dependence of Luminescence and Decay Time under Optical Excitation from Li₆Gd(BO₃)₃:Ce Single Crystals [J]. Journal of Inorganic Materials, 2007, 22(1): 25-29.
[12]	LI Jin,CHEN Zhen-Hua. C/C Composites Fabricated by the Chemical Liquid Phase Vaporization Densification with the Catalyst [J]. Journal of Inorganic Materials, 2005, 20(6): 1450-1456.
[13]	XIAO Hai-Bin,HU Guan-Qin,XU Li. Influence of Temperature Gradient on Radiation Damage of BGO Crystals [J]. Journal of Inorganic Materials, 2003, 18(2): 470-474.