金属卤化物钙钛矿半导体器件在高能辐射探测中的研究进展与应用

张至涵; 雷雨田; 靳志文

doi:10.7498/aps.75.20260817

金属卤化物钙钛矿半导体器件在高能辐射探测中的研究进展与应用

兰州大学, 兰州大学物理科学与技术学院, 兰州理论物理中心, 甘肃省理论物理重点实验室, 量子理论及应用基础教育部重点实验室, 甘肃省量子物理基础学科研究中心, 兰州　730000

通讯作者: E-mail: leiyt19@lzu.edu.cn.; E-mail: jinzw@lzu.edu.cn.

Metal halide perovskite semiconductor devices for high-energy radiation detection: Recent progress and applications

Gansu Provincial Research Center for Basic Disciplines of Quantum Physics, Key Laboratory of Theoretical Physics of Gansu Province, Key Laboratory of Quantum Theory and Applications of MoE, Lanzhou Center for Theoretical Physics, School of Physical Science and Technology, Lanzhou University, Lanzhou 730000, China

Corresponding authors: E-mail: leiyt19@lzu.edu.cn.; E-mail: jinzw@lzu.edu.cn.

摘要: 高能辐射(包括α粒子、β粒子、γ射线、中子及X射线)的高效探测能力, 直接关系到核安全监控、医学影像诊断、高能物理实验、工业无损检测及空间探索等国家战略与民生关键领域的技术水平. 近年来, 金属卤化物钙钛矿材料因其有效原子序数大、载流子输运性能优异、能带和组分可调、光致发光量子产率高等优势, 在高能辐射探测领域展现出巨大的应用潜力. 本文基于金属卤化物钙钛矿材料在五类高能辐射探测中取得的最新研究进展, 系统综述了钙钛矿半导体器件在上述5个方向的具体应用突破, 涵盖了经典三维、二维和其他低维钙钛矿等多种材料体系, 总结了当前研究面临的主要挑战, 并针对性地提出了若干改进策略与未来发展方向.
- 钙钛矿 /
- 高能辐射探测 /
- 辐射探测器
Abstract: High-energy radiation detection, covering α particles, β particles, γ rays, neutrons, and X-rays, is of critical importance for numerous strategic and societal fields, including nuclear safety monitoring, medical imaging, high-energy physics experiments, industrial nondestructive evaluation, and space exploration. Nevertheless, conventional semiconductor and scintillation detectors still encounter considerable challenges associated with limited detection efficiency, insufficient energy resolution, complex fabrication processes, and difficulties in large-area integration and flexible device development. Therefore, the exploration of novel semiconductor materials with high radiation sensitivity, efficient charge transport, and tunable device functionalities has become increasingly important.Metal halide perovskites have recently attracted extensive attention as promising materials for next-generation radiation detection owing to their unique combination of high effective atomic numbers, strong radiation absorption capability, excellent carrier transport characteristics, long carrier diffusion lengths, large carrier mobility-lifetime products (μτ), defect tolerance, and highly tunable chemical compositions and electronic structures. These intrinsic advantages enable perovskite-based semiconductor devices to achieve remarkable progress in both direct charge-collection detectors and indirect scintillation-based detection systems.In this review, we systematically summarize the recent advances in metal halide perovskite semiconductor devices for high-energy radiation detection. First, the fundamental interaction mechanisms between different radiation types and semiconductor materials are introduced, including energy deposition, electron–hole pair generation, carrier transport, and signal conversion processes for α particles, β particles, γ rays, neutrons, and X-rays. Subsequently, the key performance parameters for evaluating radiation detectors are comprehensively discussed, including the carrier mobility-lifetime product (μτ), sensitivity, energy resolution, detection efficiency, and response time. The relationships between material properties, device structures, and detector performance are further analyzed to provide a comprehensive understanding of performance optimization strategies.Furthermore, recent achievements of perovskite-based radiation detectors are reviewed according to different radiation detection scenarios. Three-dimensional perovskites, two-dimensional layered perovskites, and other low-dimensional perovskites have demonstrated outstanding potential through advances in crystal growth, defect regulation, compositional engineering, interface modification, and device architecture optimization. In particular, perovskite detectors have achieved significant breakthroughs in γ-ray and X-ray detection due to their high atomic-number constituents, excellent charge collection capability, and superior radiation interaction efficiency. Meanwhile, emerging applications in α-particle, β-particle, and neutron detection highlight the versatility of perovskite materials in complex radiation environments and multifunctional detection systems.Finally, the current challenges and future perspectives of metal halide perovskite radiation detectors are discussed, with particular emphasis on long-term operational stability, lead toxicity, scalable crystal growth, reproducible fabrication, interface engineering, and practical device integration. Future developments combining advanced material design, defect management, device engineering, and environmentally sustainable strategies are expected to further promote the transition of perovskite radiation detectors from laboratory demonstrations toward practical applications in high-performance, flexible, and multifunctional radiation sensing platforms.
- perovskite /
- high-energy radiation detection /
- radiation detectors .

图 1 (a) α粒子在空气中传播时的散射与能量损失示意图^[29]; (b) FAPbBr₃单晶的α粒子直接探测系统框图^[30]; (c)内建电场或反向偏压下用于载流子的收集器件结构^[31]; (d) α粒子间接探测系统示意图^[32]; (e) β粒子与固体通过非弹性散射相互作用产生连续信号的示意图; (f)入射β粒子与原子核发生弹性散射以及与核外电子发生非弹性散射的示意图; (g)入射β粒子散射的示意图^[22]; (h) γ光子与探测器之间的相互作用: 光电效应、康普顿散射和电子对效应^[24]; (i) γ射线与探测器之间四种主要相互作用的示意图^[25]; (j)间接探测与直接探测的探测机制^[33]; (k) CsPbBr₃探测器(直接型探测器)示意图^[34]; (l)间接型探测器示意图^[35]

Figure 1. (a) Schematic diagram of scattering and energy loss of α-particles propagating in air^[29]; (b) block diagram of the direct α-particle detection system based on FAPbBr₃ single crystal^[30]; (c) device configuration for carrier collection under built-in electric field or reverse bias^[31]; (d) schematic diagram of the indirect α-particle detection system^[32]; (e) schematic illustration of sequential signals produced by the interactions between β particles and solids via inelastic scattering; (f) schematic view of elastic scattering with nucleus and inelastic scattering with extranuclear electrons for incident β particles; (g) schematic presentation of the scattering events of incident β particles^[22]; (h) interactions between gamma photons and the detector: photoelectric effect, Compton scattering, and pair production^[24]; (i) sketch of the four main interactions between γ-rays and the detector^[25]; (j) detection mechanisms of indirect and direct detection^[33]; (k) schematic diagram of a CsPbBr₃ detector (direct-type detector)^[34]; (l) schematic diagram of an indirect-type detector^[35].

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图 2 (a) BGaN探测器(无转换层探测器)原理示意图; (b)有转换层的探测器原理示意图^[38]; (c)热中子入射到含有放射性核素(如¹⁰B和⁶Li)的钙钛矿变体材料中, 发生核反应, 产生γ射线和重带电粒子, 如α粒子^[46]; (d)快中子入射到杂化钙钛矿材料中, 与氢原子相互作用, 发生核反冲反应产生质子; (e) (PEA)₂PbBr₄快中子探测原理示意图^[47]; (f)直接型探测法与间接型探测法的对比^[42]; (g)高能X射线发生能量沉积的方式; (h)直接型探测的能带图; (i)高能光子辐照下半导体中电子(e^–)-空穴(h⁺)产生的机制; (j)间接探测路径中, 电子(e^–)和空穴(h⁺)向发光中心输运过程的示意图; (k)高能辐射与钙钛矿之间相互作用过程的基本特征、二次电子的形成过程以及热化过程^[4]

Figure 2. (a) Schematic diagram of the detection principle of a BGaN detector (converter-free detector); (b) schematic diagram of the detection principle of a detector with a converter layer^[38]; (c) thermal neutrons incident on variants of perovskite containing radionuclides (e.g., ¹⁰B and ⁶Li) undergo nuclear reactions, generating γ-rays and heavy charged particles such as α-particles^[46]; (d) fast neutrons incident on hybrid perovskite interact with hydrogen atoms, resulting in nuclear recoil reactions that produce protons; (e) schematic diagram of the fast neutron detection principle of (PEA)₂PbBr₄^[47]; (f) comparison between direct and indirect X-ray detection methods^[42]; (g) energy deposition mechanisms of high-energy X-rays; (h) energy band diagram of direct detection; (i) mechanism of electron (e^–)-hole (h⁺) generation in semiconductors under high-energy photon irradiation; (j) schematic diagram of the transport process of electrons (e^–) and holes (h⁺) toward luminescent centers in an indirect detection pathway; (k) basic features of interaction processes between high-energy radiation and perovskites, formation process of secondary electrons, and thermalization process^[4].

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图 3 (a)不同晶体厚度下的CsPb₂Br₅相缺陷和CsPbBr₃与CsPb₂Br₅的结构对比图^[29]; (b) TOPCON结构硅基集成金属卤化物钙钛矿探测器的器件架构示意、截面形貌、高分辨透射电镜晶格像及界面元素能谱分布表征^[31]; (c) FPB单晶生长设备的示意图; (d) FPB单晶钙钛矿闪烁体探测器结构图; (e) DPSI两性离子的分子结构; (f) FPB钙钛矿的晶体结构以及DPSI与钙钛矿的相互作用; (g)使用DPSI生长的抛光后的FPB单晶; (h) DPSI单晶的偏振光显微镜(PLM)图像和DPSI:LS单晶的PLM图像^[59]; (i) (PEA)₂PbI₄的晶胞结构; (j) (PEA)₂PbI₄单晶的成核控制型单晶生长过程示意图^[60]; (k)由各组分固态合成CsPbBr₃及制备自立式PS-CsPbBr₃复合薄膜的示意流程^[61]

Figure 3. (a) The CsPb₂Br₅ phase defects at different crystal thicknesses and The structure of CsPbBr₃ and CsPb₂Br₅^[29]; (b) device schematic, cross-sectional SEM, HR-TEM lattice image, and EDS elemental mapping of TOPCON-silicon-based integrated metal halide perovskite detectors^[31]; (c) a schematic diagram of the crystal growth setup; (d) the overall FPB SC device structure; (e) Molecular structure of the DPSI zwitterion; (f) the crystal structure of the FPB perovskite and the interaction of the DPSI with the perovskite; (g) a polished FPB SC grown with the DPSI additive; (h) PLM image of the DPSI SC. and PLM image of the DPSI:LS SC^[59]; (i) Crystal unit cell structure of (PEA)₂PbI₄; (j) schematic diagram of the nucleation-controlled single crystal growth process of (PEA)₂PbI₄^[60]; (k) schematic representation of the solid-state synthesis of CsPbBr₃ from its constituents and the fabrication of free-standing PS-CsPbBr₃ composite films^[61].

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图 4 (a)闪烁测试系统装置的示意图; (b)获得的图案; (c) STA₂PbBr₂的水相合成示意图; (d) STA₂PbBr₂薄膜的接触角测试图^[22]; (e)使用4×4像素化CsPbBr₃探测器的钙钛矿γ相机对锝–99m(^99mTc)γ射线成像的示意图; (f)结合机械抛光和DMSO刻蚀处理后的晶体表面(比例尺: 0.2 mm)和仅经机械抛光处理的晶体表面的脉冲高度分布图^[65]; (g) (PEA)₂PbBr₄单晶可见光下的照片、XRD图谱、上表面的SEM图像和横截面的SEM图像; (h) (PEA)₂PbBr₄单晶在α粒子(²⁴¹Am)和γ射线(¹³⁷Cs)激发下的响应时间以及在²⁴¹Am和¹³⁷Cs源辐照下α/γ甄别的散点图; (i) D-D混合辐射场下的n/γ甄别散点图以及相同条件下以距离为横坐标的n/γ分辨率直方图^[68]; (j) ITC过程的示意图及生长的CCI单晶样品^[69]; (k)安瓿瓶中$\phi$12—13 mm的单晶, 在254 nm激发下, 安瓿瓶内未掺杂的Cs₃(Cu_1–xLi_x)₂I₅和(Cs_1–xLi_x)₃Cu₂I₂晶体以及在自然白光下安瓿瓶内的Tl掺杂晶体; (l)在自然白光下, 未掺杂和Tl掺杂的Cs₃(Cu_1–xLi_x)₂I₅及(Cs_1–xLi_x)₃Cu₂I₂的抛光样品; 样品中的Li浓度从左到右递增^[70]

Figure 4. (a) Illustration of the setup of the system for scintillation test; (b) the obtained patterns; (c) diagrammatic presentation of the aqueous synthesis of STA₂PbBr₂; (d) contact angle test of the STA₂PbBr₂ film^[22]; (e) a schematic illustration of 99 mTc γ-ray imaging by perovskite γ-ray camera using 4×4 pixelated CsPbBr₃ detectors; (f) crystal surface processed by a combination of mechanical polishing and DMSO etching (scale bar: 0.2 mm); and pulse height mapping of crystal surface processed by only mechanical polishing^[65]; (g) photograph under visible light, XRD pattern, top-surface SEM image, and cross-sectional SEM image of (PEA)₂PbBr₄ single crystal; (h) response time of (PEA)2 PbBr4 SC under α particles (²⁴¹Am)and γ-rays (¹³⁷Cs) excitation and the scatter plot for α/γ discrimination under the irradiation of ²⁴¹Am and ¹³⁷Cs source; (i) the n/γ discrimination scatter plot under the D-D mixed radiation field and the n/γ resolution histogram with distance as the abscissa under the same conditions^[68]; (j) schematics of the ITC process and grown CCI single-crystal samples^[69]; (k) $\phi$12–13 mm single crystals of undoped Cs₃(Cu_1–xLi_x)₂I₅ and (Cs_1–xLi_x)₃Cu₂I₂ inside the ampules under 254 nm excitation and Tl-doped crystals inside the ampules under natural white light; (l) polished samples of undoped and Tl-doped Cs₃(Cu_1–xLi_x)₂I₅ and (Cs_1–xLi_x)₃Cu₂I₂ under natural white light, Li concentrations in the samples increased from left to right^[70].

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图 5 (a) BDAPbBr₄的晶体结构; (b) BDAPbBr₄探测器的快中子成像结果^[73]; (c) MHyPbCl₃的结构示意图^[74]; (d) (PEA)₂PbBr₄二维杂化钙钛矿的分子结构示意图; (e)快中子辐照实验的装置示意图和柔性二维钙钛矿探测器的实物照片^[75]; (f)用于测量中子响应的测试装置; (g)用于n/γ甄别及中子能量分辨的TOF方法^[47]; (h)整个(PEA)₂PbBr₄单晶生长过程的流程图^[76]; (i)基于核反冲过程(主要为弹性散射)的富氢闪烁体与利用核反应过程(³⁵Cl(n, p)³⁵S)的Cs₅Cu₃Cl₆I₂闪烁体用于快中子成像的性能比较; (j)中国散裂中子源(CSNS)快中子成像系统的原理图及工作原理; (k)由聚四氟乙烯(PTFE)构成的N形中空圆柱体的快中子图像. 插图为该圆柱体在明场下的横截面照片^[77]

Figure 5. (a) Crystal structure of BDAPbBr₄; (b) the fast-neutron imaging result by BDAPbBr₄ detector^[73]; (c) structure schematic of MHyPbCl₃^[74]; (d) the molecular structure of the (PEA)₂PbBr₄ 2D hybrid perovskite; (e) schematic diagram of the fast neutron irradiation experimental setup and photograph of the flexible 2D perovskite-based detector^[75]; (f) the testing setup for the measurement of neutron response; (g) the TOF method for n_f/γ discrimination and neutron energy resolution^[47]; (h) flow chart of the entire(PEA)₂PbBr₄ single crystal growth process^[76]; (i) comparison of fast neutron imaging performance between hydrogen-rich scintillators based on the nuclear recoil process (predominantly elastic scattering) and Cs₅Cu₃Cl₆I₂ scintillators utilizing the nuclear reaction process (³⁵Cl(n, p)³⁵S); (j) schematic and operating principles of the fast neutron imaging system at CSNS; (k) fast neutron image of an N-shaped hollow cylinder composed of PTFE, the inset shows the cross-sectional photograph of the cylinder in bright-field^[77].

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图 6 (a) MAPbI₃晶格结构示意图; (b)氘代MA⁺(氘原子以红色表示)与八面体笼中I^–(Pb以黄色表示, I以紫色表示)之间形成的3个氢键示意图, PbI₆八面体及周围8个MA⁺的示意图^[79]; (c) FAPbBr₃晶体探测器结构示意图; (d)预处理过程前(左)与过程中(右) $ \text{V}_{\text{Br}}^{+} $的分布情况^[66]; (e)沿b轴方向观察的堆积结构^[82]; (f) BiCuSCl₂的(左)价带顶(VBM)和(右)导带底(CBM)态的电荷密度分布图; (g) BiCuSCl₂X射线探测器的X射线成像测量示意图^[83]; (h)尺寸为4.60 cm×3.80 cm的大面积透明(PEA)₂PbBr₄单晶^[60]; (i) H-Cl晶体的合成路线示意图, 单晶结构, 堆积排列方式, 以及H-Cl的模拟与实验PXRD图谱^[84]; (j) Cs₂NaTbCl₆ DPSCs的水热合成示意图及其三维立方结构; (k) Cs₂NaTbCl₆薄膜在日光、紫外光下及弯曲状态下的照片. 不同种类物体在Cs₂NaTbCl₆薄膜上的X射线图像, 不同模型在Cs₂NaTbCl₆薄膜上的成像示意图^[85]

Figure 6. (a) Schematic diagram of the MAPbI₃ lattice structure; (b) schematic diagram of three hydrogen bonds formed between deuterated MA⁺ (D atom in red) and I^– in octahedral cages of Pb (yellow) and I (purple), schematic diagram of PbI₆ octahedron and eight surrounding MA^+[79]; (c) illustration ofFAPbBr3 crystal detector structure; (d) distribution of $ \text{V}_{\text{Br}}^{+} $ before (left) and during (right) the preconditioning process^[66]; (e) packing structure viewed along the b-axis^[82]; (f) charge density plots of (left)valence band maximum (VBM)and (right) conduction band minimum (CBM)states for BiCuSCl₂; (g) schematic of X-ray imaging measurement of the BiCuSCl₂ X-ray detector^[83]; (h) the photograph of a large-area transparent (PEA)₂PbBr₄ SC with dimensions of 4.60 cm×3.80 cm^[60]; (i) schematic diagram of the synthetic route for H-Cl crystals, single crystal structure, the packing arrangement, and simulated and experimental PXRD patterns of H-Cl^[84]; (j) schematic illustration of hydrothermal synthesis of Cs₂NaTbCl₆ DPSCs and 3D cubic structure of Cs₂NaTbCl₆ DPSCs; (k) photographs of the Cs₂NaTbCl₆ film under sunlight, UV light, and bending. X-ray images of different types of objects (the patterned metal sheet, the circuit board, the capsule) on the Cs₂NaTbCl₆ film; imaging diagram of different models on the Cs₂NaTbCl₆ film^[85].

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表 1 金属卤化物钙钛矿材料体系分类及其在高能辐射探测中的应用特点

Table 1. Classification of metal halide perovskite material systems and their characteristics for high-energy radiation detection.

材料体系	代表材料	结构特征	优势	高能辐射探测应用
经典三维钙钛矿	CsPbX₃, MAPbX₃, FAPbX₃等	三维ABX₃连续八面体结构, 载流子迁移率高、扩散长度长	μτ积高、缺陷密度低、能量分辨率高	X射线、γ射线、 α粒子、β粒子
二维钙钛矿	A₂PbX₄, APbX₄(A代表一价或二价尺寸较大的有机胺阳离子)	层状结构, 具有量子限域效应	稳定性高、暗电流低、可实现自驱动探测	X射线、中子探测、柔性探测、自驱动探测
其他低维钙钛矿	包含各类零维或一维结构, 没有统一的结构组成式	无机骨架呈一维链状或孤立存在, 结构组成容易调控	可溶液加工、结构可调性高、光电性能优异	在X射线、中子探测 (有机阳离子含氢多)

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1. 引　言

高能辐射包括α粒子、β粒子、γ射线、中子及X射线等, 这些辐射的能量高、穿透能力强、电离密度大, 能够与物质发生复杂的相互作用, 产生可探测的物理信号, 在核物理研究、空间科学探测、医学影像诊断、工业无损检测、核安全监控以及国防安全等领域发挥着不可替代的作用^[1,2].

根据辐射探测方式的不同, 钙钛矿高能辐射探测器可分为直接型和间接型(闪烁体型)两大类. 在直接探测模式下, 高能辐射直接与钙钛矿半导体材料相互作用, 通过电离激发产生电子-空穴对, 并在外加电场作用下被电极收集, 形成电信号. 在间接探测模式下, 钙钛矿材料作为闪烁体, 先将高能辐射转换为紫外或可见光光子, 再经过光电探测器转换为电信号. 两种探测模式各有优劣. 直接探测器结构相对简单、能量分辨率高、响应速度快, 器件结构紧凑, 但对材料的质量与电极工艺要求更高; 间接探测器易于大面积集成、与现有成像系统兼容, 但能量分辨率通常低于直接探测器. 在实际应用中, 可根据具体探测场景来选择或组合使用两种探测模式^[3–6].

随着核技术的发展与应用, 对高能辐射探测技术提出了更高的要求, 要实现高灵敏度、高能量分辨率、低检测限、高响应速度、大尺寸制备, 还要在高温、高湿、强辐照的环境中能够稳定运行^[7]. 传统辐射探测材料, 如硅(Si)、锗(Ge)等半导体探测器, 虽然具有较高的能量分辨率, 但原子序数较低, 对高能γ射线和中子的探测效率有限^[8]; 碲锌镉(CdZnTe, CZT)等化合物半导体探测器虽在γ能谱探测中性能优越, 但制备工艺复杂、成本较高且难以实现大面积集成^[9]; 传统闪烁体材料(如NaI:Tl, CsI:Tl, BGO等)可实现大尺寸制备, 但存在光产额不足、能量分辨率较低、易潮解等问题^[10]. 因此, 开发新型辐射探测材料, 成为当前高能辐射探测领域的研究重点和挑战.

近年来, 金属卤化物钙钛矿(下文简称钙钛矿)作为优异的半导体材料在光电器件和核电子领域备受关注. 钙钛矿材料的通用化学式为ABX₃, 其中A位通常是半径较大的阳离子(FA, MA或Cs等), B位是半径较小的过渡金属或主族金属阳离子(Pb, Bi等), X位为卤素离子(Cl, Br, I等)或赝卤素离子(SCN^–, $ \text{PF}_{4}^{-} $等). 在该结构中, BX₆八面体构成了钙钛矿的骨架结构, B位金属阳离子的s/p轨道与X位卤素离子的p轨道发生杂化, 形成离域化程度较高的能带结构, 使载流子具有较小的有效质量和较高的迁移率^[11]. 同时, 钙钛矿材料中的多数本征缺陷能级多为浅能级, 降低了非辐射复合的概率, 有利于载流子的长距离输运与收集^[12–15]. 基于上述结构与电子特性, 钙钛矿材料在高能辐射探测领域展现出如下优势: 1)钙钛矿材料的有效原子序数(Z_eff)较大(例如CsPbBr₃的Z_eff约为68), 显著高于Si(14)和Ge(32), 因而辐射吸收能力更强, 并且通过组分调控(如卤素替换、A位离子替代)可进一步优化其吸收特性. 2)钙钛矿材料的载流子迁移率-寿命积(μτ积)大, 载流子在复合前能够被有效收集, 提高了探测灵敏度和能量分辨率. 3)通过组分和维度调控, 可调节禁带宽度、激子结合能、载流子有效质量及发光特性, 适配不同的辐射探测场景. 4)与传统Si, Ge及CdZnTe等半导体材料相比, 钙钛矿材料制备工艺更简单, 成本更低^[3,16–18].

正是基于优异的辐射吸收能力和载流子输运特性, 钙钛矿材料近年在高能辐射探测领域备受关注. 基于钙钛矿材料的辐射探测研究开始于2015年, MAPbI₃单晶实现X射线的直接探测^[19]. 此后, 随着高质量钙钛矿单晶和薄膜制备技术的不断成熟, 以及缺陷调控、界面工程和器件结构优化等的发展, 钙钛矿探测器的性能不断提升, 研究范围也逐渐由X射线和γ射线探测拓展至α粒子、β粒子及中子等多种辐射类型, 形成了直接探测与闪烁体探测两种体系, 并在灵敏度、能量分辨率、响应时间等方面展现出显著优势.

本文主要综述了近年来钙钛矿在高能辐射探测领域的研究进展. 首先介绍了五种辐射与钙钛矿作用的机制, 接着阐述了高能辐射探测器件的主要性能指标, 并重点综述了近年来钙钛矿材料在不同辐射类型探测中的应用, 最后对钙钛矿材料高能辐射探测方面的发展趋势与未来改进方向进行了展望.

3. 性能指标

3.1. 载流子迁移率-寿命乘积(μτ积)

载流子迁移率-寿命乘积(μτ积)是表征半导体材料辐射探测能力的关键参数, 定义为载流子迁移率μ和载流子寿命τ的乘积^[48]. μτ积越大, 辐射作用后产生的电子-空穴对在复合前能够迁移的有效距离越长, 电荷收集效率(CCE)越高, 器件输出的总电荷也就越多. 因此, μτ积会影响信号幅值和能谱峰型. 晶体中μτ积分布均匀的器件信号涨落更小. 影响μτ积的因素较多, 主要有陷阱态密度、复合速率、晶体缺陷和离子迁移, 电场强度也会影响μτ积的大小.

3.2. 灵敏度(S)

灵敏度描述器件对单位剂量高能辐射信号的响应强度, 能够衡量器件探测弱高能辐射的能力, 定义式为^[43]S = (I_ray–I_dark)/(DA), 其中I_dark表示暗电流, I_ray是射线照射下的输出电流, D为辐射剂量率, A为有效面积. 影响灵敏度的因素主要有材料对射线的吸收效率、电荷收集效率和晶体质量.

3.3. 能量分辨率(ER)

能量分辨率指器件区分不同辐射能量的能力, 是能谱分析的基础, 直观体现是能谱中全能峰的尖锐程度. ER越小, 能量分辨能力越强, 可由以下公式来计算^[49]: ER = FWHM/E×100%, 其中, FWHM是全能峰的半高宽, 反映信号的涨落范围, 涨落越小, FWHM就越窄; E为峰值能量. ER的主要影响因素同样有电荷收集效率和晶体质量. 此外, 电子学噪声也是影响器件ER的主要因素之一. 在没有信号输入时, 自身会产生随机电信号波动, 造成干扰, 使分辨能力降低.

3.4. 探测效率(ε)

探测效率决定器件对入射辐射的响应能力, 是描述器件将入射辐射粒子转化为可记录的电信号能力的物理量. 器件的ε可由以下公式来计算^[50]: ε_in = C_R/C_i, $ {\varepsilon }_{\text{in}} $为固有探测效率, C_R为探测器实际记录的粒子数, C_i为实际入射到探测器灵敏区的粒子总数. 粒子进入器件后的物理过程为: 粒子入射→与探测器材料相互作用→能量沉积→产生次级粒子→信号收集与识别→有效计数, 在每个环节均可能发生能量损失. 影响器件探测效率的因素有μτ积、材料原子序数、器件尺寸和辐射的能量与类型等.

3.5. 响应时间

响应时间用于描述探测器对入射辐射信号产生电学响应的快慢, 是探测器对入射辐射产生电信号并恢复至初始状态所需的时间. 响应时间越短, 说明探测器能够越快地完成载流子的产生、输运和收集, 更适用于高速辐射成像. 响应时间分为上升时间和下降时间两部分, 上升时间为输出信号由稳态值的10%增至90%所需的时间, 下降时间为信号由90%衰减到10%所需的时间. 载流子的渡越时间可表示为^[51] t_tr = L²/(μV), 其中, L是器件厚度, μ是载流子迁移率, V是外加偏压. 该公式表明, 提高迁移率或增大偏压均可以缩短载流子渡越时间, 提升器件响应速度. 器件的响应时间还受陷阱态与缺陷密度的影响. 材料中的缺陷、杂质和晶界会形成陷阱态, 俘获载流子, 需要经过一定时间才能重新释放, 从而延长响应时间.

金属卤化物钙钛矿半导体器件在高能辐射探测中的研究进展与应用

通讯作者: E-mail: leiyt19@lzu.edu.cn.; E-mail: jinzw@lzu.edu.cn.

Metal halide perovskite semiconductor devices for high-energy radiation detection: Recent progress and applications

Corresponding authors: E-mail: leiyt19@lzu.edu.cn.; E-mail: jinzw@lzu.edu.cn.

计量

金属卤化物钙钛矿半导体器件在高能辐射探测中的研究进展与应用

通讯作者: E-mail: leiyt19@lzu.edu.cn.;

通讯作者: E-mail: jinzw@lzu.edu.cn.

English Abstract