低维卤化物钙钛矿直接型X射线探测器研究进展

doi:10.15541/jim20230016

无机材料学报 ›› 2023, Vol. 38 ›› Issue (9): 1017-1030.DOI: 10.15541/jim20230016 CSTR: 32189.14.10.15541/jim20230016

所属专题：【信息功能】敏感陶瓷（202409）；【能源环境】钙钛矿(202409)

低维卤化物钙钛矿直接型X射线探测器研究进展

董思吟¹(), 帖舒婕¹, 袁瑞涵¹^,², 郑霄家¹^,²()

1.中国工程物理研究院化工材料研究所, 绵阳 621900
2.四川省新材料研究中心, 成都 610200

收稿日期:2023-01-10 修回日期:2023-03-27 出版日期:2023-09-20 网络出版日期:2023-04-11
通讯作者: 郑霄家, 副研究员. E-mail: xiaojia@caep.cn
作者简介:董思吟(1997-), 男, 博士研究生. E-mail: 1450063752@qq.com
基金资助:
四川省科技创新人才(2022JDRC0021);国家自然科学基金(NSFC62004182)

Research Progress on Low-dimensional Halide Perovskite Direct X-ray Detectors

DONG Siyin¹(), TIE Shujie¹, YUAN Ruihan¹^,², ZHENG Xiaojia¹^,²()

1. Institute of Chemical Materials, China Academy of Engineering Physics, Mianyang 621900, China
2. Sichuan Research Center of New Materials, Chengdu 610200, China

Received:2023-01-10 Revised:2023-03-27 Published:2023-09-20 Online:2023-04-11
Contact: ZHENG Xiaojia, associate professor. E-mail: xiaojia@caep.cn
About author:Dong Siyin (1997-), male, PhD candidate. E-mail: 1450063752@qq.com
Supported by:
Sichuan Science and Technology Program(2022JDRC0021);National Natural Science Foundation of China(NSFC62004182)

摘要/Abstract

摘要：

X射线探测在医学影像、安检、工业无损探测等领域应用广泛。卤化物钙钛矿X射线探测器因具有灵敏度高、检测下限低等显著优点而引人瞩目, 然而三维结构的钙钛矿内部离子迁移显著, 导致其稳定性较差。研究表明, 低维结构可以有效抑制钙钛矿中的离子迁移, 进而提高钙钛矿X射线探测器的稳定性。本文围绕X射线探测器的工作原理、关键性能参数、低维钙钛矿材料及器件等方面, 详细介绍了低维钙钛矿X射线探测器近期的研究进展,系统分析了低维钙钛矿材料的结构特性及其对X射线探测性能的影响。低维钙钛矿可实现兼具高灵敏度和高稳定性X射线探测器的制备, 是发展潜力巨大的候选材料。进一步优化材料体系, 设计器件结构, 制备大面积、像素化的成像器件, 深入研究探测器的工作机制等是促进低维钙钛矿X射线探测器走向应用的关键。

关键词: 低维材料, 钙钛矿, X射线探测, 综述

Abstract:

X-ray detection has been widely used in medical imaging, security inspection, and industrial non-destructive tests. Halide perovskite X-ray detectors have attracted increasing attention due to their high sensitivity and low detection limit, but the notorious ion migration leads to poor operational stability. It is reported that the low dimensional structure can effectively suppress the ion migration of perovskites, thus greatly improving the stability of the detectors. This review introduces the working mechanism, key performance parameters of perovskite X-ray detectors, and summarizes the recent progress of low-dimensional perovskite materials and their application in direct X-ray detectors. The relationship between the structural characteristics of low-dimensional perovskite materials and their X-ray detection performance was systematically analyzed. Low-dimensional perovskite is a promising candidate for the preparation of X-ray detectors with both high sensitivity and stability. Further optimization of detection material and device structure, preparation of large-area pixelated imaging devices, and study of working mechanism in-depth of the detector are expected to promote the practical application of perovskite X-ray detectors.

Key words: low-dimensional materials, perovskite, X-ray detection, review

中图分类号:

O472+

董思吟, 帖舒婕, 袁瑞涵, 郑霄家. 低维卤化物钙钛矿直接型X射线探测器研究进展[J]. 无机材料学报, 2023, 38(9): 1017-1030.

DONG Siyin, TIE Shujie, YUAN Ruihan, ZHENG Xiaojia. Research Progress on Low-dimensional Halide Perovskite Direct X-ray Detectors[J]. Journal of Inorganic Materials, 2023, 38(9): 1017-1030.

图/表 7

图1 (a)间接型和(b)直接型X射线探测的原理示意图[33⇓-35]

Fig. 1 Schematic diagram of (a) indirect and (b) direct X-ray detection[33⇓-35]

图2 不同维度卤化物钙钛矿的分子结构示意图[17]

Fig. 2 Schematic representation of the molecular structures of halide perovskites with different dimensions[17]

图3 0D铋基钙钛矿单晶探测器

Fig. 3 0D bismuth-based perovskite single crystal detector (a) Schematic crystal structure and photograph of MA3Bi2I9 single crystal[25]; (b) Photograph of the MA3Bi2I9 single crystal after cutting and polishing[25]; (c) Resistivity of representative X-ray detection materials; (d) Device operational stability against continuous X-ray irradiation with high dose rates under a high bias volage[25]; (e) Photograph and corresponding X-ray images of the keys[54]; (f) FWHM of (00l) peaks of Cs3Bi2I9 single crystals, which are prepared by liquid diffusion separation induced crystallization method and inverse temperature crystallization method[53]

图4 1D和2D铋基钙钛矿单晶探测器

Fig. 4 1D and 2D bismuth-based perovskite single crystal detectors (a) Photograph of 1D (H2MDAP)BiI5 single crystal and schematic diagram of device structure[57]; (b, c) Crystal structure of (b) 1D (DMEDA)BiI5 and (c) 2D (NH4)3Bi2I9[29,58]; (d) Photograph of the (NH4)3Bi2I9 single crystal and two different device structures based on the (100) plane[29]

图5 2D钙钛矿X射线探测器

Fig. 5 2D perovskite X-ray detectors (a) Schematic diagram of the crystal structures of RP and DJ perovskites [63]; (b) X-ray image of nut based on (BA)2PbI4 single crystal device[64]; (c) X-ray images generated by (F-PEA)2PbI4 single crystal device[66]; (d) Schematic diagram of the transition of pure 2D perovskites to quasi-2D perovskites[70]

图6 准2D多晶X射线探测器

Fig. 6 Quasi-2D polycrystalline X-ray detector (a) Preparation of RP perovskite-nylon matrix by a lamination process[26]; (b) Photograph and corresponding X-ray image of a copper Chinese characters pattern[26]; (c) A-site cation engineering to prepare RP perovskite X-ray detectors[22]; (d) Microstructure of the TFT substrate and 12×12 pixel perovskite X-ray detector[22]; (e) Images of visible light and X-rays based on BA2MA9Pb10I31 detector[22]; (f) X-ray image based on (BA2PbBr4)0.5-FAPbI3 device[83]; (g) Dark current uniformity of MAPbI3 device (left) and quasi-2D PEA2MA8Pb9I28 device (right)[84]

表1 低维钙钛矿X射线探测器性能比较

Table 1 Comparison of low-dimensional perovskite X-ray detectors

Compound	E_ph/keV, V_p/kV_p	Thickness/ mm	Electric field/ (V·mm^-1)	Sensitivity/ (µC·Gy_air⁻¹·cm⁻²)	LoD/ (nGy_air·s⁻¹)	Resistivity/ (Ω·cm)	Bandgap/ eV	µτ/ (cm²·V⁻¹)	Ref.
Single crystal
Cs₄PbI₆	30 keV	-	-	451.49	90	-	3.46	9.7×10^-4	[55]
Cs₃Bi₂I₉	40 kV_p	1.2	50	1652.3	130	2.79×10¹⁰	1.96	7.97×10^-4	[28]
Cs₃Bi₂I₉	45 keV	1	120	964	44.6	1.12×10⁹	~1.89	1.87×10^-3	[53]
MA₃Bi₂i₉	100 kV_p	2.5	48	10620	0.62	5.27×10¹¹	1.98	2.8×10^-3	[25]
MA₃Bi₂i₉	40 kV_p	1	60	1947	83	3.74×10¹⁰	1.99	2.87×10^-3	[54]
FA₃Bi₂I₉	45 keV	0.9	~560	598.1	200	7.8×10¹⁰	2.08	2.4×10^-5	[52]
(DMEDA)BiI₅	50 kV_p	0.6	494	72.5	-	-	1.82	-	[58]
(H₂MDAP)BiI₅	70 keV	2	5	1.0	-	2.1×10¹⁰	1.83	-	[57]
CsPbI₃	50 kV_p	-	4.17	2370	3020	7.4×10⁹	2.67	3.63×10^-3	[59]
(NH₄)₃Bi₂I₉(∥001)	22 keV	-	2.2	8200	210	-	2.05	1.1×10^-2	[29]
(NH₄)₃Bi₂I₉ (⊥001)	22 keV	-	6.5	803	55	-	2.05	4.0×10^-3	[29]
Rb₃Bi₂I₉	30 keV	1	300	159.7	8.32	2.3×10⁹	1.89	2.51×10^-3	[61]
(F-PEA)₂PbI₄	120 keV	1.5	~130	3402	23	1.36×10¹²	2.30	5.1×10^-4	[66]
(PMA)₂PbI₄	40 kV_p	0.9	~56	283	2130	-	2.01	8.05×10^-3	[67]
BA₂PbI₄	30 kV_p	2	10	148	241	2.6×10¹¹	2.24	4.5×10^-4	[64]
BA₂CsPbBr₇	40 kV_p	3.91	2.53	13260	72.5	2.2×10⁹	2.74	-	[68]
BA₂EA₂Pb₃Br₁₀	70 keV	2	5	6.8×10³	5500	4.5×10¹⁰	2.55	1.0×10^-2	[69]
(CH₃OC₃H₉N)₂CsPb₂Br₇	80 kV_p	2	0	410	-	-	2.51	3.2×10^-3	[70]
BDAPbI₄	40 kV_p	-	310	242	430	-	2.37	4.43×10^-4	[72]
(BDA)CsPb₂Br₇	50 kV_p	0.7	~43	725.5	3810	4.35×10¹⁰	2.76	2.33×10^-5	[73]
(3AMPY)(FA)Pb₂I₇	50 kV_p	1	200	5.23×10⁴	151	-	1.54	2.0×10^-3	[75]
Polycrystalline
MA₃Bi₂i₉	35.5 keV	1	210	563	9.3	2.28×10¹¹	2.08	4.6×10^-5	[77]
MA₃Bi₂i₉	30.6 keV	~0.1	150	~35	140	~5×10¹¹	2.09	3.89×10^-5	[78]
MA₃Bi₂i₉	30.6 keV	~0.05	600	~100	98.4	3.38×10¹¹	2.03	1.6×10^-6	[79]
MA₃Bi₂i₉	40 kV_p	0.1	2000	2065	2.71	3.5×10⁸	1.86	-	[80]
Cs₄PbBr₆	-	0.3	666.7	7068	1.75	1.376×10¹¹	3.88	1.01×10^-3	[81]
Cs₂TeI₆	40 kV_p	0.025	25	19.2	-	4.2×10¹⁰	1.57	5.2×10^-5	[82]
BA₂MA₉Pb₁₀I₃₁	~60 keV	0.9	110	5362.3	8.1	~1×10¹⁰	~1.60	3.99×10^-5	[26]
BA₂MA₉Pb₁₀I₃₁	45 keV	1	210	7109	9.3	~1.1×10¹⁰	~1.61	~5×10^-5	[22]
(BA₂PbBr₄)_0.5FAPbI₃	-	0.006	~167	1.36×10⁴	4.2	-	-	-	[83]
PEA₂MA₈Pb₉I₂₈	50 kV_p	-	600	10 860	69	5.4×10¹⁰	1.504	2.6×10⁻⁵	[84]

表1 低维钙钛矿X射线探测器性能比较

Table 1 Comparison of low-dimensional perovskite X-ray detectors

Compound	E_ph/keV, V_p/kV_p	Thickness/ mm	Electric field/ (V·mm^-1)	Sensitivity/ (µC·Gy_air⁻¹·cm⁻²)	LoD/ (nGy_air·s⁻¹)	Resistivity/ (Ω·cm)	Bandgap/ eV	µτ/ (cm²·V⁻¹)	Ref.
Single crystal
Cs₄PbI₆	30 keV	-	-	451.49	90	-	3.46	9.7×10^-4	[55]
Cs₃Bi₂I₉	40 kV_p	1.2	50	1652.3	130	2.79×10¹⁰	1.96	7.97×10^-4	[28]
Cs₃Bi₂I₉	45 keV	1	120	964	44.6	1.12×10⁹	~1.89	1.87×10^-3	[53]
MA₃Bi₂i₉	100 kV_p	2.5	48	10620	0.62	5.27×10¹¹	1.98	2.8×10^-3	[25]
MA₃Bi₂i₉	40 kV_p	1	60	1947	83	3.74×10¹⁰	1.99	2.87×10^-3	[54]
FA₃Bi₂I₉	45 keV	0.9	~560	598.1	200	7.8×10¹⁰	2.08	2.4×10^-5	[52]
(DMEDA)BiI₅	50 kV_p	0.6	494	72.5	-	-	1.82	-	[58]
(H₂MDAP)BiI₅	70 keV	2	5	1.0	-	2.1×10¹⁰	1.83	-	[57]
CsPbI₃	50 kV_p	-	4.17	2370	3020	7.4×10⁹	2.67	3.63×10^-3	[59]
(NH₄)₃Bi₂I₉(∥001)	22 keV	-	2.2	8200	210	-	2.05	1.1×10^-2	[29]
(NH₄)₃Bi₂I₉ (⊥001)	22 keV	-	6.5	803	55	-	2.05	4.0×10^-3	[29]
Rb₃Bi₂I₉	30 keV	1	300	159.7	8.32	2.3×10⁹	1.89	2.51×10^-3	[61]
(F-PEA)₂PbI₄	120 keV	1.5	~130	3402	23	1.36×10¹²	2.30	5.1×10^-4	[66]
(PMA)₂PbI₄	40 kV_p	0.9	~56	283	2130	-	2.01	8.05×10^-3	[67]
BA₂PbI₄	30 kV_p	2	10	148	241	2.6×10¹¹	2.24	4.5×10^-4	[64]
BA₂CsPbBr₇	40 kV_p	3.91	2.53	13260	72.5	2.2×10⁹	2.74	-	[68]
BA₂EA₂Pb₃Br₁₀	70 keV	2	5	6.8×10³	5500	4.5×10¹⁰	2.55	1.0×10^-2	[69]
(CH₃OC₃H₉N)₂CsPb₂Br₇	80 kV_p	2	0	410	-	-	2.51	3.2×10^-3	[70]
BDAPbI₄	40 kV_p	-	310	242	430	-	2.37	4.43×10^-4	[72]
(BDA)CsPb₂Br₇	50 kV_p	0.7	~43	725.5	3810	4.35×10¹⁰	2.76	2.33×10^-5	[73]
(3AMPY)(FA)Pb₂I₇	50 kV_p	1	200	5.23×10⁴	151	-	1.54	2.0×10^-3	[75]
Polycrystalline
MA₃Bi₂i₉	35.5 keV	1	210	563	9.3	2.28×10¹¹	2.08	4.6×10^-5	[77]
MA₃Bi₂i₉	30.6 keV	~0.1	150	~35	140	~5×10¹¹	2.09	3.89×10^-5	[78]
MA₃Bi₂i₉	30.6 keV	~0.05	600	~100	98.4	3.38×10¹¹	2.03	1.6×10^-6	[79]
MA₃Bi₂i₉	40 kV_p	0.1	2000	2065	2.71	3.5×10⁸	1.86	-	[80]
Cs₄PbBr₆	-	0.3	666.7	7068	1.75	1.376×10¹¹	3.88	1.01×10^-3	[81]
Cs₂TeI₆	40 kV_p	0.025	25	19.2	-	4.2×10¹⁰	1.57	5.2×10^-5	[82]
BA₂MA₉Pb₁₀I₃₁	~60 keV	0.9	110	5362.3	8.1	~1×10¹⁰	~1.60	3.99×10^-5	[26]
BA₂MA₉Pb₁₀I₃₁	45 keV	1	210	7109	9.3	~1.1×10¹⁰	~1.61	~5×10^-5	[22]
(BA₂PbBr₄)_0.5FAPbI₃	-	0.006	~167	1.36×10⁴	4.2	-	-	-	[83]
PEA₂MA₈Pb₉I₂₈	50 kV_p	-	600	10 860	69	5.4×10¹⁰	1.504	2.6×10⁻⁵	[84]

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低维卤化物钙钛矿直接型X射线探测器研究进展

Research Progress on Low-dimensional Halide Perovskite Direct X-ray Detectors

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