辐射光致发光材料及其应用研究进展

doi:10.15541/jim20220677

无机材料学报 ›› 2023, Vol. 38 ›› Issue (7): 731-749.DOI: 10.15541/jim20220677 CSTR: 32189.14.10.15541/jim20220677

辐射光致发光材料及其应用研究进展

李乾利¹(), 黎乃鑫¹, 李育成¹, 刘慎业², 程帅³, 杨光¹, 任宽²(), 王峰², 赵景泰¹^,³()

1.上海大学材料科学与工程学院, 上海 200444
2.中国工程物理研究院激光聚变研究中心, 绵阳 621050
3.桂林电子科技大学广西电子信息材料构效关系重点实验室, 桂林 541004

收稿日期:2022-11-14 修回日期:2022-12-27 出版日期:2023-02-21 网络出版日期:2023-02-21
通讯作者: 任宽, 副研究员. E-mail: yunlongrk1990@sina.com;
赵景泰, 教授. E-mail: jtzhao@guet.edu.cn
作者简介:李乾利(1989-), 男, 博士, 副教授. E-mail: liqianli@shu.edu.cn
基金资助:
国家自然科学基金(11905122);国家自然科学基金(11805184);中国工程物理研究院院长基金(YZJJLX2019011);中国工程物理研究院激光聚变研究中心青年人才基金攀登基金(RCFPD4-2020-1);广西科技基地和人才专项(2020AC18005);中央引导地方科技发展资金专项(桂科ZY22096009)

Research Progress of Radio-photoluminescence Materials and Their Applications

LI Qianli¹(), LI Naixin¹, LI Yucheng¹, LIU Shenye², CHENG Shuai³, YANG Guang¹, REN Kuan²(), WANG Feng², ZHAO Jingtai¹^,³()

1. School of Materials Science and Engineering, Shanghai University, Shanghai 200444, China
2. Laser Fusion Research Center, China Academy of Engineering Physics, Mianyang 621050, China
3. Guangxi Key Laboratory of Information Materials, Guilin University of Electronic Technology, Guilin 541004, China

Received:2022-11-14 Revised:2022-12-27 Published:2023-02-21 Online:2023-02-21
Contact: REN Kuan, associate professor. E-mail: yunlongrk1990@sina.com;
ZHAO Jingtai, professor. E-mail: jtzhao@guet.edu.cn
About author:LI Qianli (1989-), male, PhD, associate professor. E-mail: liqianli@shu.edu.cn
Supported by:
National Natural Science Foundation of China(11905122);National Natural Science Foundation of China(11805184);President's Foundation of China Academy of Engineering Physics(YZJJLX2019011);Youth Talent Foundation of Laser Fusion Research Center of China Academy of Engineering Physics(RCFPD4-2020-1);Guangxi Science and Technology Base and Talent Special Project(2020AC18005);Central Government Guided Local Science and Technology Development Fund Project(ZY22096009)

摘要/Abstract

摘要：

随着我国核辐射技术的进步, 辐射探测在近些年也得到了高速发展, 并被广泛应用于辐射安全监测、放射性医学诊疗、X射线安监系统、工业无损探伤以及微观粒子轨迹探测等诸多领域。辐射光致发光(Radio- photoluminescence, RPL)是一种在电离辐射作用下, 材料内部产生新的发光中心, 并被紫外光激发进而发光的现象, 可作为一种新型辐射探测手段。RPL材料通常具有存储辐射信息、信息几乎不衰减、剂量线性响应好、均匀稳定的高辐射灵敏度、能量依赖性小和可重复读数等特点, 弥补了光释光(Optically stimulated luminescence, OSL)和热释光(Thermally stimulated luminescence, TSL)材料在存储稳定性和重复使用性等方面的不足。自RPL现象被报道以来, RPL材料层出不穷, 如传统的Ag掺杂磷酸盐玻璃、Al₂O₃:C,Mg和LiF, 再到新型的Cu离子掺杂体系、Sm离子掺杂体系以及无掺杂体系材料等。同时, RPL应用也被不断发掘, 目前它已成为辐射探测领域不可或缺的材料之一。基于此, 本文概述了RPL材料的最新进展, 重点梳理了传统和新型RPL材料的发光原理、性能特点及其应用, 特别对比了不同RPL材料在辐射探测性能方面的差异。最后, 本文对RPL材料的优势及其不足之处进行了归纳分析, 并对其发展趋势进行了展望。

关键词: 辐射光致发光, 辐射探测, 剂量监测, Ag掺杂磷酸盐玻璃, X射线成像

Abstract:

With the progress of nuclear radiation technology in China, radiation detection has been developed rapidly in recent years for the wide usage in radiation safety monitoring, radioactive medicine diagnosis/treatment, X-ray security inspection, industrial non-destructive detection, microscopic particle track detection, and many other fields. Radio-photoluminescence (RPL), as a new radiation detection method, is a phenomenon in which a new luminescence center is generated inside a material under a ionizing radiation which can be excited by ultraviolet light to emit a special light. RPL materials usually have characteristics of storing radiation information, almost no attenuation of information, good linear dose response, high radiation sensitivity, low energy dependence, and repeatable reading, which can overcome the shortcomings in stability and reusability of optically stimulated luminescence (OSL) materials and thermally stimulated luminescence (TSL) materials. Since the RPL phenomenon was reported, RPL materials have emerged constantly, from the traditional materials as Ag-doped phosphate glass, Al₂O₃:C, Mg and LiF, to the novel materials such as Cu-doped RPL system, Sm-doped RPL system and undoped RPL system materials. Meanwhile, applications of RPL materials have also been explored, enabling them to become one of the indispensable materials in the field of radiation detection. Based on above aspects, this paper summarizes the latest development of RPL materials, focuses on the luminescence principle, performance characteristics and applications of traditional and novel RPL materials, and especially compares the performance of different RPL materials in radiation detection. Finally, advantages and disadvantages, accompanied by prospected development trend of RPL materials are summarized and analyzed

Key words: radio-photoluminescence, radiation detection, dose detection, Ag-doped phosphate glass, X-ray imaging

中图分类号:

TQ174

李乾利, 黎乃鑫, 李育成, 刘慎业, 程帅, 杨光, 任宽, 王峰, 赵景泰. 辐射光致发光材料及其应用研究进展[J]. 无机材料学报, 2023, 38(7): 731-749.

LI Qianli, LI Naixin, LI Yucheng, LIU Shenye, CHENG Shuai, YANG Guang, REN Kuan, WANG Feng, ZHAO Jingtai. Research Progress of Radio-photoluminescence Materials and Their Applications[J]. Journal of Inorganic Materials, 2023, 38(7): 731-749.

图/表 9

图1 RPL材料及其应用

Fig. 1 RPL materials and their applications The central area is a general luminescence diagram of RPL materials, the central ring area introduces common and new RPL materials, and the outer ring area lists some potential applications of RPL materials. FNTD: fluorescent nuclear track detector

图2 三种通用发光机制的示意图以及Ag离子掺杂材料、Al2O3:C,Mg和LiF的RPL响应及其RPL中心

Fig. 2 Schematic diagram of three general luminescence mechanism, and RPL responses and RPL centers of Ag-doped materials, Al2O3:C,Mg and LiF (a) Schematic diagram of RPL/OSL/TSL general luminescence mechanisms[13]; (b) Excitation and emission spectra of Ag-PG[7]; (c) Emission spectra of Ag-PG under different doses of X-ray irradiation[51]; (d) Excitation spectrum (pink dotted line) and emission spectrum of Ag-Rb glass before and after X-ray (10 Gy) irradiation[53]; (e) Emission spectra of Ag-Nd co-doped phosphate glass at different radiation doses (310 nm excitation)[54]; (f) Excitation spectrum (dashed line) and emission spectrum (solid line) of Ag-doped CsCl before and after X-ray irradiation[58]; (g) Excitation and emission contour spectra of Al2O3:C,Mg irradiated by β-rays (90Sr/90Y)[61]; (h) Excitation spectrum and emission spectrum of LiF after X-ray irradiation (126 Gy)[62]; (i) RPL defect center in LiF, where F3+ is formed by three anionic vacancies capturing two electrons and F2 is formed by two anionic vacancies capturing two electrons[7]; Colorful figures are available on website

表1 不同种类的RPL材料

Table 1 Different kinds of RPL materials

No.	Material	Material form^a	RPL center	λ_em/mm	λ_ex/mm	Sensitivity/Gy	Build-up	Ref.
1	NaPO₃-Al(PO₃)₃:Ag	Glass	Ag⁰,	400-500	325/339	1×10^-6-10	Yes^b	[22-24]
1	NaPO₃-Al(PO₃)₃:Ag	Glass	Ag²⁺, Ag₂⁺	600-700	325/339	1×10^-6-10	Yes^b	[22-24]
2	LiPO₄-Al(PO₃)₃:Ag	Glass	Ag²⁺	630	340			[25]
3	KPO₃-Al(PO₃)₃:Ag	Glass	Ag²⁺	550-700	300-350	0.1-10		[26]
4	P₂O₅-Al₂O₃-Na₂O-SiO₂:Ag	Glass	Ag⁰	460	310	0.1×10^-3-10	Yes	[27]
4	P₂O₅-Al₂O₃-Na₂O-SiO₂:Ag	Glass	Ag²⁺, Ag₂⁺	630	310	0.1×10^-3-10	Yes	[27]
5	NaCl:Ag	S.C	Ag⁰	550-650	289			[28]
5	NaCl:Ag	S.C	Ag⁰	500-600	339			[28]
6	KCl:Ag	S.C	Ag⁰	400-550	289			[28]
6	KCl:Ag	S.C	Ag⁰	500-700	339			[28]
7	Al₂O₃:C,Mg	S.C.	F⁺(Mg)	325	255	2×10^-3-200	Yes	[11,19, 29]
			F₂	500	300
			F₂⁺(2Mg)	750	355
			F₂²⁺(2Mg)	510	435
8	LiF:Mg	S.C.	F₃⁺, F₂	530	450	0.1-1.4×10⁴	Yes	[30]
9	MgF₂:Sm	P.C.	Sm²⁺	700-800	340	1-1×10³	No	[31]
10	SrB₄O₇:Sm	P.C.	Sm²⁺	670-830	408	0.2-5×10³		[32]
11	BaAlBO₃F₂:Sm	G.C.	Sm²⁺	670-850	300-500	0.01-10	No	[33]
12	CaSO₄:Sm	P.C.	Sm²⁺	600-900	300	0.015-5	No	[34]
13	Ca₂SiO₄:Eu	P.C.	Eu²⁺	500-800	250-500	0.01-10		[35]
14	BaAlBO₃F₂:Eu	G.C.	Eu²⁺	510	300-450	0.02-10	Yes	[36]
15	KCaPO₄:Eu	P.C.	Eu²⁺	610	200-500	0.01-10		[37]
15	KCaPO₄:Eu	P.C.	Eu²⁺	490	350	0.01-10		[37]
16	90KPO₃-10Al₂O₃:Ce	S.C.	Ce³⁺	300-400	310	1×10^-5-1		[38]
17	NaCl:Yb	S.C.	Yb²⁺	425-430	200-400	0.1-100		[39]
18	C:N	S.C. film	NV	689	546		Yes	[40]
19	SiO₂-B₂O₃-Al₂O₃-Na₂O:Cu	Glass	Cu⁺	500-800	240	~500	Yes	[41]
20	MgF₂	P.C.		415	340	100-1000	Yes	[42]
20	MgF₂	P.C.		700	340	100-1000	Yes	[42]
21	CaF₂	S.C.	F₂⁺	660	370/560			[43]
21	CaF₂	S.C.	(F₂⁺)_A	760	390/610			[43]
22	CaF₂:Na	S.C.	(F₂⁺)_A	750	390/610	1×10^-5-10		[44]
22	CaF₂:Na	S.C.	F₃	950	450/610	1×10^-5-10		[44]
23	Li₂CO₃	P.C.		470	340	1×10^-5-0.1		[45]
24	K₂CO₃	P.C.		440	340	1×10^-3-10		[46]
25	CaSO₄	P.C.		690	590	4×10^-4-5	No	[47]

图3 Cu离子掺杂材料的RPL现象及其响应

Fig. 3 RPL and its responses of Cu-doped materials (a) Photos of undoped, 0.005% and 0.01% Cu-doped (in mole fraction) aluminoborosilicate glass under natural and ultraviolet light (254 nm) with brown part of the glass being exposed to X-ray[41]; (b) Emission spectra of undoped and doped aluminoborosilicate glass at 240 nm excitation before and after X-ray irradiation[41]; (c) Relationship between PL intensity and irradiation (or absorption) dose of 0.005% Cu-doped aluminumborosilicate glass irradiated by γ-ray (60Co)[41]; (d) Effect of heat treatment on X-ray irradiated 0.005% Cu-doped aluminoborosilicate glass[41]; (e) Emission spectra of Cu-doped silica glass before and after γ-ray irradiation at 240 nm excitation[64]; (f) Emission spectra of Cu-doped silica glass before and after irradiation with γ-rays (1519 Gy) with emission band after irradiation containing two bands of 2.5 and 2.1 eV (blue line)[64]; (g) Fitting curve of the relationship between PL intensity and radiation dose of Cu-doped silica glass[64]; (h) Emission spectra of Cu-doped aluminoborosilicate glasses before and after X-ray irradiation at 240 nm with inset showing ABS25 (top) and ABS30 (bottom) before (left) and after (right) X-ray irradiation, respectively[65]

图4 Sm离子掺杂材料的RPL响应、重复使用性以及RPL有效性与主体材料带隙能量的关系

Fig. 4 RPL responses, reusability and effectiveness of RPL in relation to band gap energy of host in Sm-doped materials (a) Linear response lines of RPL intensity and radiation dose of Sm-doped BaF2-Al2O3-B2O3[33]; (b) Dose response curves of Sm-doped CaSO4, SrSO4, BaSO4 and commercial RPL glass dosimeter (Ag-PG)[34]; (c) Stability curves of RPL signals doped with CaSO4, SrSO4 and BaSO4 during UV excitation. The measured irradiation dose of each group was fixed at 5.0 Gy, and PL spectra were measured every minute after irradiation (20 times in total) to obtain its response value[34]; Reusability of Sm-doped RPL detectors after (d) heat treatment and (e) UV irradiation erasure[7]; (f) Effectiveness of RPL in Sm-doped RPL materials as a function of band gap energy of host[71]

图5 其他新型材料(Li2CO3、CaSO4和MOF结构)的RPL响应以及MOF的晶体结构

Fig. 5 RPL responses of other novel materials and their crystal structure of MOF (a) Emission spectra of Li2CO3 before and after X-ray (10 mGy) irradiation, with the excitation wavelength of (340±40) nm with inset showing the excitation spectrum before and after X-ray (1 Gy) irradiation at the monitoring wavelength 470 nm[45]; (b) Curve of RPL response strength of Li2CO3 ceramics with time at the excitation of (340±40) nm[45]; Excitation emission contour maps of undoped CaSO4 before (c) and after (d) X-ray irradiation (5 Gy)[47]; (e) Relationship between PL spectrum and irradiation dose of undoped CaSO4 with inset showing the dose-response function compared with commercial RPL glass detector[47]; (f) Relationship between the RPL response stability and the number of readings of CaSO4 and commercial RPL glass detectors[47]; (g) Crystal structure of SCU-200 with schematic diagrams (1)-(4) indicating crystal habit and size of a crystal (1), coordination mode of the Pb2+ ion (2), one-dimensional chain constructed from PbO7 polyhedra (3), and three-dimensional arrangement of the one-dimensional chain (4), respectively[74]; (h) Emission spectra of SCU-200 after irradiation with different doses of X-ray[74]; Colorful figures are available on website

图6 RPL材料用于辐射剂量计

Fig. 6 RPL materials for radiation dosimetry (a) Fluorescence attenuation curve (top) and novel readout technique using pulsed ultraviolet laser (bottom)[7]; (b) Internal images of RPLGD[7]; (c) Comparison of RPL response signals irradiated by different metal filters and different types of radiation (X, γ and β-rays)[7]; (d) Spherical RPLGD prepared by melting method[79]; (e) Spherical RPLGD used to monitor radioactive contaminants in harsh environments[80]; (f) 2D dose distribution of each layer at different depths of the hand model soaked in polyester resin block (left) and 3D dose distribution of the complete structure of the hand model after X-ray irradiation[83]; (g) Contrast enhanced image of RPL photograph after digital image processing with inset showing RPL glass particles covered with polystyrene plate placed in a petri dish. When the dose is higher than 5 Gy, RPL can be observed with a digital camera at a dose higher than 0.5 Gy, and when RPL glass particles were exposed to gamma rays (60Co) they can emit orange light under UV light[84]; Colorful figures are available on website

图7 RPL材料用于FNTD以及MRT

Fig. 7 RPL materials for FNTD and MRT (a) Nuclear track detection of fast neutrons demonstrated by using Al2O3:C,Mg[85]; (b) Nuclear track image obtained by using LiF as FNTD[7]; (c) Histogram of nuclear tracks detected by Al2O3:C,Mg[86]; (d) Dose response function of Sm-doped RPL materials for dose monitoring in MRT[71]

图8 RPL材料用于辐射成像

Fig. 8 RPL materials for radiation imaging (a) Microscale patterns of (1) two-dimensional code, (2) lines, circles and dots written on Ag-PG using a focused proton beam with an energy of 1.7 MeV and a current of 4 pA, (3) 3D images of dots- and lines-patterns written on Ag-PG using a focused proton beam with an energy of 1.7 MeV and a current of 20 pA[93]; (b) X-ray imaging of Ag-PG used in (1) medical imaging and (2) industrial nondestructive testing[95]; (c) X-ray imaging of LiCaAlF6:Sm with the micron level spatial resolution[69]; (d) X-ray imaging of BaF2-Al2O3-B2O3:Sm with a spatial resolution of 5l lp/mm (100 μm)[33]; (e) X-ray images (1) using a disk-type imaging detector with LiF film[62] with two reconstructed dose distribution images using a disk-type Ag-PG detector in (2) orange and (3) blue RPL[98]; (f) Photograph of (1) a flexible imaging plate made by using (Ba1-xSrx)2SiO4:Eu before X-ray irradiation, (2) image of the X-ray irradiated imaging plate under UV excitation with the luminous color changing from red to green, X-ray images obtained after (3) 10 and (4) 28 d at room temperature in the dark[99]

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辐射光致发光材料及其应用研究进展

Research Progress of Radio-photoluminescence Materials and Their Applications

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