微量SiO2添加对Pr:Lu3Al5O12陶瓷光学及闪烁性能的影响

doi:10.15541/jim20190418

无机材料学报 ›› 2020, Vol. 35 ›› Issue (7): 796-802.DOI: 10.15541/jim20190418 CSTR: 32189.14.10.15541/jim20190418

所属专题：功能材料论文精选(一)：光学材料(2020)

微量SiO₂添加对Pr:Lu₃Al₅O₁₂陶瓷光学及闪烁性能的影响

胡泽望^1,²,陈肖朴^1,²,刘欣^1,²,李晓英^1,²,石云¹,寇华敏¹,谢腾飞¹,李江^1,²()

1. 中国科学院上海硅酸盐研究所, 透明光功能无机材料重点实验室, 上海 201899
2. 中国科学院大学材料与光电研究中心, 北京100049

收稿日期:2019-08-13 修回日期:2019-09-30 出版日期:2020-07-20 网络出版日期:2019-12-04
作者简介:胡泽望(1992-), 男, 博士研究生. E-mail: huzewang@student.sic.ac.cn
HU Zewang(1992-), male, PhD candidate. E-mail: huzewang@student.sic.ac.cn
基金资助:
国家重点研发计划项目(2017YFB0310502);国家重点研发计划项目(2016YFB0701004);国家自然科学基金(61775226);国家自然科学基金(61675221)

Trace SiO₂ Addition on Optical and Scintillation Property of Pr:Lu₃Al₅O₁₂ Ceramics

HU Zewang^1,²,CHEN Xiaopu^1,²,LIU Xin^1,²,LI Xiaoying^1,²,SHI Yun¹,KOU Huamin¹,XIE Tengfei¹,LI Jiang^1,²()

1. Key Laboratory of Transparent Opto-functional Inorganic Materials, Shanghai Institute of Ceramics, Chinese Academy of Sciences, Shanghai 201899, China
2. Center of Materials Science and Optoelectronics Engineering, University of Chinese Academy of Sciences, Beijing 100049, China

Received:2019-08-13 Revised:2019-09-30 Published:2020-07-20 Online:2019-12-04
Supported by:
National Key R&D Program of China(2017YFB0310502);National Key R&D Program of China(2016YFB0701004);National Natural Science Foundation of China(61775226);National Natural Science Foundation of China(61675221)

摘要/Abstract

摘要：

在制备透明陶瓷时, 广泛采用烧结助剂来提升陶瓷的光学质量。但烧结助剂的添加可能会恶化陶瓷的发光性能。本研究采用真空预烧结合热等静压烧结制备了0.25at%Pr:LuAG闪烁陶瓷, 研究了微量SiO₂烧结助剂对陶瓷光学及闪烁性能的影响。结果表明, 添加少于200 ppm的微量SiO₂(1 ppm表示添加量为1×10^-6 g/g)能有效促进热等静压过程中气孔的排出, 有效提升了Pr:LuAG陶瓷的光学性能。150 ppm SiO₂添加的Pr:LuAG陶瓷在400 nm处的直线透过率约为77%。同时研究了预烧温度及时间对Pr:LuAG陶瓷光学性能的影响。在实现完全闭气孔结构时, 进一步升高预烧温度或延长保温时间会降低热等静压过程中的致密化速率, 不利于气孔的排出, 从而降低了Pr:LuAG陶瓷的光学质量。此外, 添加微量SiO₂对Pr:LuAG陶瓷闪烁性能的影响较小。添加微量SiO₂结合热等静压烧结是制备Pr掺杂石榴石闪烁陶瓷的有效途径。

关键词: Pr:LuAG陶瓷, 烧结助剂, 光学质量, 闪烁性能

Abstract:

Sintering aids are widely used to improve the optical quality of ceramics in the preparation of transparent ceramics. However, sintering aids may deteriorate the luminescent properties of the ceramics. In this work, 0.25at%Pr:LuAG scintillation ceramics were prepared by vacuum pre-sintering combined with hot isostatic pressing. The influences of trace SiO₂ sintering aid on the optical and scintillation properties of the ceramics were studied. The results show that a small amount of SiO₂ below 200 ppm (1 ppm means that addition content is 1×10^-6 g/g) can effectively promote the remove of pore during hot isostatic pressing and improve the optical quality of the Pr:LuAG ceramics. Their in-line transmittance with 150 ppm SiO₂ is about 77% at 400 nm. The effects of pre-sintering temperature and holding time on the optical properties of Pr:LuAG ceramics were also investigated. When completely closed pore structure is formed, further increasing the pre-sintering temperature or prolonging the holding time reduce the densification rate in the hot isostatic pressing process, which is not conducive to the remove of pores and lower the optical quality of the Pr:LuAG ceramics. In addition, trace SiO₂ addition has less effect on scintillation properties of the Pr:LuAG ceramics. Adding trace SiO₂ sintering aid combined with hot isostatic pressing is an effective way to prepare Pr doped garnet scintillation ceramics.

Key words: Pr:LuAG ceramics, sintering aids, optical quality, scintillation property

中图分类号:

TQ174

胡泽望,陈肖朴,刘欣,李晓英,石云,寇华敏,谢腾飞,李江. 微量SiO₂添加对Pr:Lu₃Al₅O₁₂陶瓷光学及闪烁性能的影响[J]. 无机材料学报, 2020, 35(7): 796-802.

HU Zewang,CHEN Xiaopu,LIU Xin,LI Xiaoying,SHI Yun,KOU Huamin,XIE Tengfei,LI Jiang. Trace SiO₂ Addition on Optical and Scintillation Property of Pr:Lu₃Al₅O₁₂ Ceramics[J]. Journal of Inorganic Materials, 2020, 35(7): 796-802.

图/表 12

图1 不同温度预烧5 h得到的不同SiO2添加Pr:LuAG陶瓷的相对密度

Fig. 1 Relative densities of the Pr:LuAG ceramics with different SiO2 additives pre-sintered at different temperatures for 5 h

图2 不同温度预烧5 h得到的不同SiO2添加Pr:LuAG陶瓷在HIP前后的晶粒尺寸

Fig. 2 Grain size of the Pr:LuAG ceramics before and after HIP with different SiO2 additives pre-sintered at different temperatures for 5 h

图3 1775 ℃预烧5 h得到的不同SiO2添加Pr:LuAG预烧体热腐蚀表面FESEM形貌照片

Fig. 3 FESEM images of the thermally etched Pr:LuAG ceramics with different SiO2 additives pre-sintered at 1775 ℃ for 5 h (a) 0; (b) 50 ppm; (c) 100 ppm

图4 不同SiO2添加量的1775 ℃预烧5 h后Pr:LuAG陶瓷HIP后的直线透过率

Fig. 4 In-line transmittance of the HIPed Pr:LuAG ceramics pre-sintered at 1775 ℃ for 5 h with different SiO2 additives

图5 1775 ℃预烧5 h的不同SiO2添加量Pr:LuAG陶瓷HIP后热腐蚀表面及断面FESEM形貌照片

Fig. 5 FESEM images of the thermally etched surface (a-d) and fracture surface (e) of the HIPed Pr:LuAG ceramics with different SiO2 additives pre-sintered at 1775 ℃ for 5 h (a) 0 ppm; (b) 50 ppm; (c) 100 ppm; (d) 200 ppm; (e) 200 ppm

图6 不同温度预烧5 h的100 ppm SiO2添加量的Pr:LuAG陶瓷的热腐蚀表面FESEM形貌照片

Fig. 6 FESEM images of the thermally etched Pr:LuAG ceramics pre-sintered at different temperatures for 5 h with 100 ppm SiO2 additive (a) 1650 ℃; (b) 1750 ℃; (c) 1775 ℃; (d) 1800 ℃; (e) 1825 ℃

图7 不同温度预烧5 h制备的100 ppm SiO2添加量的Pr:LuAG陶瓷HIP后的直线透过率曲线

Fig. 7 In-line transmittance of the HIPed Pr:LuAG ceramics pre-sintered at different temperatures for 5 h with 100 ppm SiO2 additive

图8 不同温度预烧5 h制备的100 ppm SiO2添加量的Pr:LuAG陶瓷HIP后的热腐蚀表面FESEM形貌照片

Fig. 8 FESEM images of the thermally etched HIPed Pr:LuAG ceramics pre-sintered at different temperatures for 5 h with 100 ppm SiO2 additive (a) 1750 ℃; (b) 1775 ℃; (c)1800 ℃; (d) 1825 ℃

图9 不同SiO2添加量经1775 ℃预烧不同时间的Pr:LuAG陶瓷的致密化曲线

Fig. 9 Relative densities of the Pr:LuAG ceramics pre-sintered at 1775 ℃ with different holding time and different SiO2 additives

图10 1775 ℃预烧不同时间制备的不同SiO2添加量的Pr:LuAG陶瓷HIP后的直线透过率

Fig. 10 In-line transmittance of the HIPed Pr:LuAG ceramics pre-sintered at 1775 ℃ with different holding time and different SiO2 additives

图11 不同SiO2添加量的Pr:LuAG陶瓷归一化XEL光谱

Fig. 11 Normalized XEL spectra of Pr:LuAG ceramics with different SiO2 additives

表1 不同SiO2添加量的Pr:LuAG陶瓷光产额、能量分辨率、闪烁衰减时间及快分量含量

Table 1 Light yield, energy resolution, scintillation decay and the intensity of fast component of the Pr:LuAG ceramics with different SiO2 additives

SiO₂/ ppm	LY, ER @1 μs /(ph·MeV^-1, %)	LY, ER @6 μs /(ph·MeV^-1, %)	τ₁/ns	τ₂/ns	I_fast/%
0	13033, 18.0	18091, 17.1	23.11	1476	46.4
50	12560, 16.5	15880, 15.3	23.75	1462	57.9
100	10686, 15.4	13453, 15.1	23.35	1343	58.2
150	9965, 15.8	12574, 15.4	21.41	1334	57.5
200	10104, 14.7	12726, 14.3	23.27	1340	58.1

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微量SiO₂添加对Pr:Lu₃Al₅O₁₂陶瓷光学及闪烁性能的影响

Trace SiO₂ Addition on Optical and Scintillation Property of Pr:Lu₃Al₅O₁₂ Ceramics

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