镥基闪烁晶体的研究进展

由于高能物理实验、核医学成像、安全检查和地质探矿等领域的迫切需要,具有高密度、快衰减、高光输出和低成本等优良特性的闪烁晶体成为关注的焦点,特别是Ce~(3+)激活的镥(Lu)基化合物,其开发、研究和应用方兴未艾。简要综述了硅酸镥、氧化镥和铝酸镥等闪烁晶体的生长技术、闪烁性能和应用,并展望了镥基闪烁晶体的发展趋势。     

无机闪烁晶体及其产业化开发

在高能粒子或射线（如X射线、γ射线等）的作用下能够发出脉冲光的物体,被称为闪烁体。它是光电功能材料,被广泛用于高能物理、核物理、空间物理、核医学、地质勘探、安全检查以及国防工业等领域。闪烁体分为无机闪烁体和有机闪烁体两大类。根据形态、成份以及结构特点,可进一步将前者分为无机闪烁晶体、闪烁玻璃、闪烁陶瓷和闪烁气体,而后者可分为有机闪烁晶体、液体闪烁体和塑料闪烁体。其中,数量最多、应用最广的当推无机闪烁晶体。本文将主要介绍无机闪烁晶体及其应用以及有关晶体的开发状况,同时对无机闪烁晶体的发展趋势也将做一简要评述。     

无机闪烁薄膜的研究进展

综述了无机闪烁薄膜材料的制备与表征、发光与闪烁性质以及当前的发展和应用情况.针对X射线高分辨成像的要求,具有较高有效原子序数和较大密度的无机闪烁材料成为当今研究的热点,重点阐述了溶胶-凝胶法制备这类闪烁薄膜的研究现状,并对其今后的发展进行了展望.     

超薄Ce:YAG闪烁晶体用于高分辨X光成像

正近期,中国科学院上海光学精密机械研究所中科院强激光材料重点实验室利用提拉法生长出的高品质Ce∶YAG闪烁晶体开展了高分辨率X射线成像系统核心器件——闪烁体研制工作,成功制备了尺寸为30 mm,厚度为30~45μm的高品质闪烁晶体元件,并和中科院上海应用物理研究所合作,研制基于超薄Ce∶YAG闪烁晶体的高分辨X光探测器,实现X光辐照条件下高分辨成像。在同等实验条件下,与Crytur公司同类晶体对比,上海光机所研制的     

X射线激发Ce^3＋掺杂硼酸盐玻璃的闪烁发光

实验研究了Ｃｅ＾３＋掺杂６４Ｂ２Ｏ３－３６ＢａＯ,７５Ｂ２Ｏ３－２５Ｌａ２Ｏ３玻璃的闪烁发光。在８０ｋＶ加速电压、阳极电流为５ｍＡ的高能Ｘ射线激发下闪烁光强为同要条件下闪烁晶体Ｎａｌ（Ｔｌ）的３％～４％。对影响闪烁光输出的因素进行了分析。结果表明,Ｃｅ＾３＋的自吸收和Ｃｅ＾４＋离子的荷移吸收是降低闪烁光输出的主要因素;含镧硼硅酸盐玻璃系统可作为发展高密度玻璃有希望的系统;闪烁玻璃的制备技术对提高闪     

无机闪烁材料研究进展

闪烁材料的发展已有一百多年的历史,其中无机闪烁材料应用最广、数量最多。无机闪烁材料主要包括陶瓷闪烁材料、晶体闪烁材料和玻璃闪烁材料三大类型。闪烁材料的闪烁性能主要包括光输出、透明性、衰减速率、高能粒子阻止能力和抗辐照损伤能力等。无机闪烁材料在影像核医学诊断、高能离子探测、工业在线无损检测以及油井勘测等领域有着广泛的应用。介绍了无机闪烁材料的三大发展阶段与三大类型,对部分重要无机闪烁材料的闪烁性能做了对比,并概括了闪烁材料的应用,展望了其发展前景。     

X射线激发Ce~(3+)掺杂硼酸盐玻璃的闪烁发光

实验研究了Ce3+掺杂 6 4B2 O3- 36BaO ,75B2 O3-2 5La2 O3玻璃的闪烁发光。在 80kV加速电压、阴极电流为 5mA的高能X射线激发下闪烁光强为同样条件下闪烁晶体NaI(Tl)的 3%～ 4 %。对影响闪烁光输出的因素进行了分析。结果表明 ,Ce3+的自吸收和Ce4+离子的荷移吸收是降低闪烁光输出的主要因素 ;含镧硼硅酸盐玻璃系统可作为发展高密度玻璃有希望的系统 ;闪烁玻璃的制备技术对提高闪烁光输出起着重要作用。     

闪烁晶体材料的研究进展

闪烁晶体用于X射线和γ射线等高能粒子探测,在分子医学成像、高能物理、核物理、安全检查、材料无损探伤和地质探矿等领域有着广泛的应用。随着人们对闪烁晶体的更加深入的认识以及晶体生长技术的发展,许多已开发的闪烁晶体的性能得到优化和提高,应用范围也随之扩大,随着应用的更高要求,对闪烁晶体的综合性能要求越来越高,进一步设计、发现、开发和生长具有高密度、优良光学均匀性、高能束粒子阻止本领、高光产额、快衰减、高稳定性、低成本等综合优良性能的闪烁晶体仍然是闪烁材料研究的重点。简要综述了近年来卤化物、钨酸盐、锗(硅)酸盐、铝酸盐和硼(磷)酸盐等重要闪烁晶体材料的研究进展及其闪烁性能和应用前景。     

无机闪烁晶体的生长技术

综述了无机闪烁晶体的提拉法，下降法，热交换法，浮区法等生长技术，其中最常有和的最前两种方法。同时就某些典型的闪烁晶体讨论了上述生长技术的优缺点。     

新型闪烁体的辐照效应

介绍了新型闪烁体辐照效应的研究进展,高能物理实验中使用的闪烁晶体（如ＰＷＯ、ＧＳＯ：Ｃe、CeF3等）用于强辐照环境,要求高辐照硬度。闪本在辐照后可能产生的变化主要有效：色心的形成、光输出改变、光输出均匀性的损伤、输出噪声增加、闪烁机制的变化。辐照效应的产生主要是晶体的缺陷所致,提高闪烁体辐照硬度的主要方法有退火、漂白、掺杂、控制晶体生长条件等,本文对此均作了较系统的综述了,同时也简介了研究辐照效应的实验方法：光谱分析法、热释光法、电子顺磁共振法、正电子湮没技术。     

陶瓷闪烁材料最新研究进展

概述了透明陶瓷的研究现状及闪烁体的一些重要性能。讨论了新型陶瓷闪烁体相比闪烁单晶在成像应用中的优势 ,介绍了几种重要的陶瓷闪烁体 ,如 (Y ,Gd) 2 O3:Eu ,Pr;Gd2 O2 S :Pr ,Ce ,F ;Gd3Ga5O1 2 :Cr,Ce ;Lu2 O3:Eu ,Tb。并陶瓷闪烁体在先进医学和工业X 射线探测器CT成像中的应用和趋向进行了展望。     

Growth and characterization of polycrystalline lanthanide halide scintillators

We are exploring a novel time- and cost-efficient approach to produce robust, large-volume polycrystalline lanthanide halide scintillators using a hot wall evaporation (HWE) technique. To date, we have fabricated LaBr₃:Ce and LaCl₃:Ce films (slabs) measuring up to 7 cm in diameter and 7+ mm in thickness (20–25 cm³ in volume) on quartz substrates. These polycrystalline scintillators exhibit very bright emissions approaching those exhibited by their melt-grown crystal counterparts. Scanning electron micrographs (SEMs) and X-ray diffraction analysis confirm polycrystalline growth with columnar structures, both of which help in light piping, thereby contributing to the observed high light yields. The new scintillators also exhibit good energy resolution for γ-rays over the tested range of 60 keV (²⁴¹Am) to 662 keV (¹³⁷Cs), although they have not yet reached that of the corresponding crystals. The measured response linearity over the same energy range is comparable for both our HWE synthesized films and melt-grown commercially-available reference crystals. Similar consistency in response is also observed in terms of their decay time and afterglow behaviors. The data collected so far demonstrate that our HWE technique permits the rapid creation of scintillators with desired structural and compositional characteristics, without the introduction of appreciable defects, and yields material performance equivalent to or approaching that of crystals. Consequently, the deposition parameters may be manipulated to tailor the physical and scintillation performance of the resulting structures, while achieving a cost per unit volume that is substantially lower than that of crystals. In turn, this promises to allow the use of these novel scintillation materials in such applications as SPECT, PET, room-temperature radioisotope identification and homeland security, where large volumes of materials in a wide variety of shapes and sizes are needed. This paper describes our growth and testing of polycrystalline LaBr₃:Ce scintillators and provides comparative characterizations of their performance with crystals.     

Perovskite: Scintillators,direct detectors,and X-ray imagers

Halide perovskites (HPs) are used in various applications, including solar cells, light-emitting diodes, lasers, and photodetectors. These materials have recently received a great deal of attention as high-energy radiation detectors and scintillators due to their excellent light yield, mobility-lifetime product (µτ), and X-ray sensitivity. In addition, due to their solution-processability and low cost, perovskite materials could be used to produce thick perovskite films across wide areas, allowing for low-dose X-ray imaging. Perovskite-based scintillators and detectors could eventually replace commercialized products like thallium‐doped cesium iodide (CsI:Tl) and amorphous silicon (Si). Here, we review all of the key properties of HPs, the relevant terminology necessary for radiation detection and scintillation, the physical mechanisms underlying their operation, the fabrication process, and perovskite crystals and thin-films of varying dimensionality used for high-energy radiation detection. We also cover the critical issues and solutions that HPs as detectors, scintillators, and imagers face.     

Photoluminescence and scintillation properties of Al(PO3)3–CsPO3–CsBr–CeBr3 glass scintillators

Scintillators, which are widely used as radiation detectors, are phosphors that release absorbed ionizing radiation energy as ultraviolet or visible light. Inorganic glass scintillators have several advantages over inorganic crystal scintillators, such as ease of fabrication and low costs. However, unlike inorganic crystals, which can emit up to tens of thousands of photons/MeV, inorganic glasses exhibit less than several hundred photons/MeV in most cases. Here, we studied an inorganic glass scintillator that exhibits a light yield of 2700 photons/MeV, which exceeds those of previous inorganic glass scintillators with high light yields of approximately 2000 photons/MeV. The density of this material is 3.28 g/cm³, which is relatively high among glass scintillators. Moreover, a fast scintillation decay with a decay time constant of 30.0 ns was obtained and is attributed to the 5d–4f transition of Ce³⁺. Thus, this glass is suitable for gamma- and X-ray detection, thereby expanding the practical applicability of inorganic glass scintillators.

     

Radiation detector developments in medical applications: inorganic scintillators in positron emission tomography

In recent years, a number of new gamma-ray scintillators are commercially available. These scintillators are either derived from known scintillators, e.g. Lu(1-x)Y(x)AlO(3): Ce (LuYAP) from LuAlO(3):Ce and Lu(2(1-x))Y(2x)SiO(5):Ce (LYSO) from Lu(2)SiO(5):Ce or are the result of new discoveries, e.g. LaCl(3):Ce and LaBr(3):Ce. The first two materials are primarily of interest because of the relatively high detection efficiency and fast response; LYSO has found application in time-of-flight (TOF) positron-emission tomography (TOF PET) and the LuYAP-LYSO combination is used in small-animal PET. The halide scintillators have an excellent energy resolution of approximately 3% at 662 keV and they have a relatively high light yield. LaBr(3):Ce is being studied for application in TOF PET. At the same time, the search for and research on new scintillator materials are going on. For example, LuI(3):Ce is a new material with a very high light yield ( approximately 90 000 photons MeV(-1)). Other examples of new materials are (C(6)H(13)NH(3))(2)PbI(4) and (C(3)H(7)NH(3))(2)PbBr(4), organic-inorganic hybrid compounds, of which the former has a very fast sub-nanosecond response. The new scintillators show great promise for new developments in medical applications, in particular, for PET systems.     

Free carrier absorption in self-activated PbWO4 and Ce-doped Y3(Al0.25Ga0.75)3O12 and Gd3Al2Ga3O12 garnet scintillators

Nonequilibrium carrier dynamics in the scintillators prospective for fast timing in high energy physics and medical imaging applications was studied. The time-resolved free carrier absorption investigation was carried out to study the dynamics of nonequilibrium carriers in wide-band-gap scintillation materials: self-activated led tungstate (PbWO₄, PWO) ant two garnet crystals, GAGG:Ce and YAGG:Ce. It was shown that free electrons appear in the conduction band of PWO and YAGG:Ce crystals within a sub-picosecond time scale, while the free holes in GAGG:Ce appear due to delocalization from Gd³⁺ ground states to the valence band within a few picoseconds after short-pulse excitation. The influence of Gd ions on the nonequilibrium carrier dynamics is discussed on the base of comparison the results of the free carrier absorption in GAGG:Ce containing gadolinium and in YAGG without Gd in the host lattice.     

Comparative study of ceramic and single crystal Ce:GAGG scintillator

Recent study revealed that single crystal Ce:Gd₃(Al,Ga)₅O₁₂ (Ce:GAGG) showed good scintillation response under γ-ray exposure. We discover here that ceramic Ce:GAGG scintillator exhibited better performance than the single crystal counterpart. We developed Ce 1% doped ceramic and single crystal GAGG scintillators with 1 mm thick and compared their properties. In radioluminescence spectra, they showed intense emission peaking at 530 nm due to Ce³⁺ 5d–4f transition. The ¹³⁷Cs γ-ray induced light yields of ceramic and single crystal resulted 70 000 ph/MeV and 46 000 ph/MeV with primary decay times of 165 and 143 ns, respectively. At present, the observed light yield was the brightest in oxide scintillators.     

La（Ce）Br3闪烁晶体的研究历史及存在的问题

最近20年来,对于无机闪烁晶体,尤其是卤化物闪烁晶体的研究而言是一段收获颇丰的历史,这期间,先后研究发现了大量光输出高、能量分辨率好、衰减时间短的新型卤化物闪烁晶体。着重介绍La(Ce)Br3晶体的研究现状以及对晶体结构、发光机制、闪烁性能和最新研究进展进行系统整理和总结,同时指出在La(Ce)Br3晶体研究中急需解决的难题、发展方向和潜在的应用前景。     

Gd3(Al,Ga)5O12:Ce闪烁晶体扭曲生长、组分偏析与性能研究

新型闪烁晶体Gd₃(Al,Ga)₅O₁₂:Ce(简写为GAGG:Ce)在制备过程中易出现多晶扭曲生长、组分偏析等问题, 严重影响晶体的性能。为了得到大尺寸高质量的GAGG:Ce晶体, 采用X射线衍射(XRD)、电感耦合等离子体发射光谱(ICP-OES)和X射线激发发射谱(XEL)等手段, 结合熔体特性分析了GAGG:Ce晶体多晶扭曲生长、组分偏析的形成机制。通过调整温场、抑制组分挥发等方法生长出φ50 mm×120 mm的GAGG:Ce晶体, 并重点研究了GAGG:Ce晶体的光谱特性与闪烁性能。结果表明: GAGG:Ce晶体的光输出达58000 ph./MeV, 能量分辨率为6.4%@662 keV, 在550~800 nm波长区间的透过率约为82%。晶体闪烁衰减快分量为126 ns (83%), 慢分量为469 ns (17%)。晶体的发射峰中心波长在550 nm左右, 与硅光电倍增管的接收波长匹配, 且发光峰值处的透过率EWLT(Emission Weighted Longitudinal Transmittance)值高达79.8%。GAGG:Ce晶体兼具高光输出与高能量分辨率, 在中子和伽马射线探测领域具有广阔的应用前景。