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摘要:
闪烁玻璃由于制备工艺简单，尺寸灵活可控，成本低廉等优点，有望成为中国环形正负电子对撞机(CEPC)中强子量能器的候选材料。其中，以Ce3+发光中心掺杂闪烁玻璃有较好的闪烁性能。玻璃基质可以分为氧化物玻璃、卤化物玻璃和微晶玻璃。本文根据Ce3+掺杂不同玻璃基质分类，重点关注了Ce3+掺杂闪烁玻璃的光学透过率、光产额、衰减时间等闪烁性能和抗辐照特性。并且，总结了国内外以及闪烁玻璃合作组的最新研究成果。针对不同玻璃体系的研究现状，从玻璃组成与制备工艺等两个方面探讨了玻璃性能提升手段。最后，对Ce3+掺杂闪烁玻璃未来的研究发展方向做出了展望。
Abstract:Scintillation glasses have potential application in hadron calorimeter of circular electron positron collider (CEPC) due to the advantages of simple preparation process, flexible and controllable size, and low cost. Among them, Ce3+ luminescent center doped scintillation glasses have better scintillation performance. Matrix glass can be classified into oxide glass, halide glass, and glass-ceramic. According to the classification of different matrix glasses, this paper focuses on the optical transmittance, light yield, decay time, and radiation resistance properties of the Ce3+-doped scintillation glasses. Moreover, we introduce and summarize the research progress at domestic, foreign, and GS R&D Group. In view of the research status of different glasses, the methods for improving the glass performance are discussed from two aspects of glass composition and preparation. Finally, the future research and development directions of Ce3+-doped scintillation glasses are prospected.
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Key words:
- hadron calorimeter /
- scintillation glass /
- Ce3+ luminescent center /
- scintillation
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Overview: Nowadays, scintillation glass has attracted worldwide attention and plays an important role in medical imaging, high energy physics, environmental monitoring, and security inspection. Scholars are exploring the application prospects of scintillation glass in high energy physics and other fields. At present, the maximum light yield of the Ce3+-doped scintillating glass can reach 4300 ph/MeV, and the maximum density can exceed 6.9 g/cm3.
With the rapid development of high energy physics, the concept of circular electron positron collider (CEPC) has been proposed. The structure of scintillation glass and silicon photomultiplier (SiPM) may be used in hadron calorimeter of CEPC. It requires a large density (>6 g/cm3) and considerable scintillation performance (light yield >1000 ph/MeV, decay time <100 ns). Among them, the Ce3+-doped glasses have better scintillation properties.
In this paper, the glasses are divided into oxide glasses, halide glasses, and glass ceramics according to the different substrates doped with Ce3+. Moreover, we focus on the optical transmittance, light yield, decay time, and irradiation resistance of the Ce3+-doped scintillation glasses. Moreover, we introduce and summarize the research progress at domestic, foreign, and GS R&D Group. In view of the research status of different glasses, the methods for improving the glass performance are discussed from two aspects of glass composition and preparation. Finally, the future research and development directions of Ce3+-doped scintillation glass are prospected.
In order to improve the scintillation performance of the glasses, future preparation methods and research directions can focus on 1) reducing impurities in glass raw materials through further purification to reduce defects in the glass; 2) Add an appropriate amount of clarifying agent and improving the glass stirring process to reduce the bubbles in the glass; 3) using a reducing atmosphere and a appropriate reducing agent to avoid the oxidation of Ce ions; 4) Partial fluoride can be used to replace the oxide to reduce the melting point of the glass, reduce the introduction of impurities in the corundum crucible, and improve the uniformity of the glass; 5) Reduce the introduction of elements that are unfavorable to scintillation performance in glass, and increase the proportion of Gd element in the glass. Exploring suitable scintillation glass components and glass preparation processes is the key to the long-term development and real application of scintillation glass in the future.
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图 3 (a) 铝硼硅酸盐玻璃和BGO晶体在137Cs (662 keV)放射源下的能谱；(b) 余辉曲线
Figure 3. (a) The energy spectra of aluminoborosilicate glass and BGO crystal under 137Cs (662 keV) source; (b) Afterglow curve
图 4 Ce3+掺杂Gd2O3–Al2O3–SiO2闪烁玻璃和BGO晶体的XEL光谱(a)和 137Cs能谱(b)
Figure 4. Scintillation properties of Gd2O3–Al2O3–SiO2 glasses, (a) the XEL spectra, (b) energy spectra (137Cs) of the glasses and BGO crystal
图 5 (a) K2O–Y2O3–Gd2O3–SiO2微晶玻璃在137Cs (662 keV)放射源下的与BGO晶体的能谱；(b) 闪烁衰减时间曲线
Figure 5. (a) The energy spectra of K2O–Y2O3–Gd2O3–SiO2 glass ceramic under 137Cs (662 keV) source with BGO crystal; (b) The scintillation decay time curve
表 1 闪烁玻璃性能参数
Table 1. Performance parameters of scintillation glass
参数 Parameter Abbreviations 密度 Density Den. 发射峰 Emission peak EP 量子产率 Quantum yield QY 光致发光衰减时间 Photoluminescence decay time PL DT 闪烁衰减时间 Scintillation decay time Sc. DT 光产额 Light yield LY 能量分辨率 Energy resolution ER 
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表 2 Ce3+掺杂硼酸盐玻璃的性能参数
Table 2. Performance parameters of Ce3+-doped borate glasses
Num. Den./(g/cm3) EP/nm QY/% PL DT/ns Sc. DT/ns LY/(ph/MeV) ER/% B-1 3.8 400 42 36 / / / B-2 / 360 50 33.4 27.2 / / B-3 3.4 360 70.1 37.89 40.1, 270.8 1800 / B-4 / 360 82 38 42, 202 256 / B-5 / 380 / 37.63 - / /
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表 3 Ce3+掺杂硅酸盐玻璃的性能参数
Table 3. Performance parameters of Ce3+-doped silicate glasses
Num. Den./(g/cm3) EP/nm QY/% PL DT/ns Sc. DT/ns LY/(ph/MeV) ER/% S-1 4.2 430 / 43.9, 73.8 90.8, 415.6 2500 / S-2 / 420 2 3 3.5 700 / S-3 4.4 431 / / 522 3460 14 S-4 / 410 20 38.1 109 / / S-5 4.5 430 / 44, 89 93, 317 2000 /
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表 4 Ce3+掺杂硼硅酸盐玻璃的性能参数
Table 4. Performance parameters of Ce3+-doped borosilicate glasses
Num. Den. /(g/cm3) EP/nm QY/% PL DT/ns Sc DT/ns ER/% BS-1 4.9 420 / / 400 / BS-2 3.9 403 / 26.6 / / BS-3 / 350 8 30.8 64 / BS-4 2.4 368 / 40 / /
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表 5 Ce3+掺杂卤化物玻璃的性能参数
Table 5. Performance parameters of Ce3+-doped halide glasses
Num. Den./(g/cm3) EP/nm QY/% PL DT/ns Sc. DT/ns LY/(ph/MeV) H-1 6.9 325 / 5.5, 23.4 / / H-2 6.0 325 / 33.2 8, 25 150 H-3 4.6 367 / 35 37 97.2 H-4 / 330 58.7 35.4 34.9, 203.7 93 H-5 / 350 75.7 26.1 24.0 23
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表 6 Ce3+掺杂微晶玻璃的性能参数
Table 6. Performance parameters of Ce3+-doped glass ceramics
Num. Den./(g/cm3) EP/nm QY/% PL DT/ns Sc. DT/ns LY/(ph/MeV) ER/% GC-1 2.45 / / / / 240% GS20 / GC-2 / 397 / 42 / / / GC-3 / 370 / 33 / / / GC-4 / 420 / 38.2 / / /
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表 7 合作组研制的闪烁玻璃性能
Table 7. Performance of scintillation glass developed by R&D group
Num. Den./(g/cm3) EP/nm PLDT/ns Sc.DT/ns LY/(ph/MeV) ER/% GS-1 4.5 390 41.69 262.1, 1234.8 802 26.8 GS-2 4.2 430 63.44 346.3, 1740.1 1206 23.0 GC-1 3.2 380 53.6 / 853 22.3 GC-2 3.3 380 / 210.4, 1622.0 1601 27.3
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