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Advanced Electronic Materials · 2018 ·Vol. 4 ·期 11 ·1800237 · IF 5.466

Ultrafast Ionizing Radiation Detection by p–n Junctions Made with Single Crystals of Solution-Processed Perovskite

Xin Wang,Yao Wu,Guanwen Li,Jun Wu,XiaoBing Zhang,Qing Li,Baoping Wang,Jing Chen,Wei Lei

Organometallic perovskites are candidates for low-dose ionizing radiation due to their large mobility-lifetime product, large radiation absorption coefficient, high stability at ambient temperature, and ability to crystallize from solution at low temperatures. However, multiple unstable and expansive organic layers are required to block injected charges from the applied voltage. Here, a radiation photodiode based on p–n junctions formed in the CH 3 NH 3 PbI 3 crystallization process without any other organic layers is reported. Through controlling the location of the dopant, selenium (Se), and its concentration inside CH 3 NH 3 PbI 3 single crystals, the valence band offset of the band alignment is measured as 0 to 0.45 eV. The photodiodes require only two gold electrodes deposited on opposite faces of the CH 3 NH 3 PbI 3 single crystals, and the sensitivity for 60 keV X-ray and 1.25 MeV gamma-ray from Cobalt-60 reached 21 µC mGy air cm −2 and 41 µC Gy air cm −2 , respectively. Experiments measured the ultrafast response time to be 3 µs.

研究领域: 材料科学 · 辐射物理学
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Journal of Materials Chemistry A · 2018 ·Vol. 6 ·期 46 ·23388-23395 · IF 9.931

Optical and electronic anisotropies in perovskitoid crystals of Cs3Bi2I9 studies of nuclear radiation detection

Qihao Sun,Yadong Xu,Hongjian Zhang,Bao Xiao,Xin Liu,Jiangpeng Dong,Yuanbo Cheng,Binbin Zhang,Wanqi Jie,Mercouri G. Kanatzidis

The halide perovskitoid compound Cs3Bi2I9 (CBI) has attracted considerable interest as a semiconductor because of its outstanding stability and reduced toxicity compared with lead-based halide perovskites. Here, we report the growth of nuclear radiation detection grade CBI bulk crystals (Φ 15 × 60 mm3) with a high resistivity of over 1010 Ω cm using a modified vertical Bridgman method. Because of their layered crystal structures we investigated the anisotropy in the optical and electrical properties using different crystal orientations. The CBI(001) sample exhibits a resistivity of ∼1012 Ω cm compared to ∼1010 Ω cm for the CBI(100) sample. This is due to the anisotropic mobility in the two crystallographic directions. Using 425 nm LED (∼200 mW cm−2) illumination CBI(001) possesses a superior optical response with a switching ratio of over 40, which is critically higher than that of CBI(100) (<2). Detectors of 2 mm thickness show a capability of detecting 241Am@5.49 MeV α particles, with good peak discrimination. A full width at half maximum (FWHM) of 32% was obtained under a bias of 560 V. Simultaneously, the electron mobility and mobility lifetime (μτ) were calculated to be 6.10 cm2 V−1 s−1 and 2.03 × 10−5 cm V−1, respectively. First-principles density functional theory calculations confirm the crystallographic anisotropy of the carrier effective masses. In addition, a significant X-ray sensitivity of 111.9 μC Gy−1 cm−2 for a CBI detector was observed, under 80 kVp X-rays at an electrical field of 450 V cm−1.

研究领域: 材料科学 · 物理学
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CRYSTAL GROWTH & DESIGN · 2024 · IF 3.2

Reverse Temperature Solution to Grow High-Quality CsCu2I3 Single Crystal with Formic Acid for Radiation Detection

Jianming Lai,Lujia Yang,Wenzhen Wang,Shaohan Wang,Yingshen Lu,Feng Hong,Fei Xu,Junfeng Chen,Yan Zhu,Hui Zhang,Run Xu,Linjun Wang

One-dimensional (1D) CsCu2I3 single crystals (SCs) have been investigated as novel sensitive X-ray and γ-ray scintillators, which can be prepared by the Bridgman method and solution method. However, to date, no research team has studied the scintillation performance of CsCu2I3 single crystals grown using the solution method, and traditionally grown single crystals using the antisolvent method are of poor quality and small sizes. In this work, high-quality CsCu2I3 SC was synthesized with formic acid as an additive by using the inverse temperature crystallization solution method, and its optical properties and scintillation performance were measured. The experimental results indicate that the addition of formic acid can stabilize the growth of crystals in solution, and the selected solvent DMF is beneficial for the growth of rod-like single crystals instead of needle-like single crystals by the DMSO. The experiment resulted in high-quality CsCu2I3 single crystals reaching a length of 13 mm, with no visible inclusions in the crystal. The full width at half-maximum (fwhm) of the X-ray rocking curve was 0.028°, indicating its high crystalline quality. It exhibits stability in air and emits bright yellow light under ultraviolet irradiation. The CsCu2I3 SC shows a much shorter PL decay of 118 ns and afterglow of 0.01% @ 12 ms compared to commercial CsI: Tl single crystal. The light yield of CsCu2I3 SC is 21800 photons/MeV, showing great potential as a scintillation material.

研究领域: 材料科学 · 物理学
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JOURNAL OF RARE EARTHS · 2024 · IF 5.2

Superdense Ce3+-activated lutetium silicate scintillating glass for radiation detection

Feng Zhang,Dazhao Wang,Guanxin Du,Hongwei Li,Dianhao Hou,Yankun Qi,Shichao Lv,Shifeng Zhou

The scintillating photonic glass has the great potential for medicine imaging, nuclear physics, high-energy physics, and national defense. However, the development of the candidate with the high density remains a significant challenge. Herein, the superdense scintillating glasses derived from the Ce 3+ -activated Lu 2 O 3 -SiO 2 binary system were successfully fabricated by the strategy of contactless aerodynamic levitation heating under the N 2 atmosphere. These glasses are colorless, optical homogeneous, and exhibit superdense density from 6.59 to 7.15 g/cm 3 , representing the highest density among the fast decay glass systems. The materials present excellent radiation-blocking ability, suitable emission wavelength, and fast response, indicating the promise for fast-event X-ray detection. The micro radiation probe was fabricated by connecting the scintillating glass and the optical fiber. The practical application in remote radiation detection is demonstrated and it exhibits excellent linear response and high signal-to-noise ratio. The results confirm that the fabricated superdense scintillating glass is promising for application in the field of high-energy radiation detection.

CAS / MDL: 1306-38-3 12032-20-1
研究领域: 材料科学 · 核物理学 · 医学成像 · 光学工程
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ACS Applied Materials & Interfaces · 2025 · IF 8.2

Centimeter-Sized CsPbBr3 Single-Crystal Films for Energy-Resolved Radiation Detection

Rong Wu,Yansong Yue,Qingya Wang,Jing Wei,Liberato Manna,Fangze Liu,Hongbo Li

Metal halide perovskites (MHPs) are promising materials for radiation detection. Compared with polycrystalline films, single crystals (SCs) have lower defect density, higher carrier mobility, and lifetime. However, the direct synthesis of MHP SCs for large-area flat panel imaging detectors remains challenging. Here, we show that high-quality centimeter-sized CsPbBr3 SCs with thicknesses between 0.25 mm and 1 mm can be grown by a space-confined inverse temperature method. The addition of choline bromide to the precursor solution reduces the defect density and suppresses ion migration of the CsPbBr3 SCs, leading to a high resistivity of 2.5 × 1010 Ω cm and a high mobility-lifetime product of over 1 × 10–3 cm2 V–1. The CsPbBr3 SC spectral detectors exhibit an energy resolution of 14.96% for 241Am 59.5 keV X-ray and 15.95% for 5.48 MeV α-particles. Moreover, a prototype 3 × 3 pixelated detector based on the large-area SC shows a consistent high performance for all pixels, making it promising for high-resolution flat panel imaging detectors.

研究领域: 材料科学 · 辐射探测技术
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CHEMISTRY OF MATERIALS · 2022 · IF 10.508

Precursor Engineering for Solution Method-Grown Spectroscopy-Grade CsPbBr3 Crystals with High Energy Resolution

Fangbao Wang,Ruichen Bai,Qihao Sun,Xin Liu,Yuanbo Cheng,Shouzhi Xi,Binbin Zhang,Menghua Zhu,Shuqing Jiang,Wanqi Jie,Yadong Xu

A CsPbBr3 single crystal exhibits great potentials in X-ray/gamma-ray spectroscopy and imaging. Here, an inverse temperature crystallization (ITC) method with modified precursor composition is proposed to prepare CsPbBr3 single crystals. The introduction of adduct PbBr2·2DMSO, synthesized by the antisolvent vapor-assisted crystallization method, in the precursor solution gives rise to superior crystallization with a lower impurity concentration and higher resistivity of 6.37 × 109 Ω·cm, as well as a higher hole mobility (50.7 cm2·V–1·s–1). Furthermore, a low dark current of 2.3 nA is obtained at a bias of −100 V based on an as-grown crystal with a thickness of 1 mm, according to the asymmetric Au/CsPbBr3/Sn structure. The resulting asymmetric planar detectors achieve the high peak-to-valley ratio pulse height spectra with an energy resolution of 7.66%, illuminated by an uncollimated 241Am@5.5 MeV α particle. Simultaneously, an energy resolution of 13.5% is realized when irradiated by a 59.5 keV 241Am γ-ray source at room temperature. The thermally stimulated current (TSC) spectra indicate that the density of deep energy-level trap is significantly reduced in the CsPbBr3 crystals grown by PbBr2·2DMSO-modified precursor solution, which is consistent with the high performance in radiation detection.

研究领域: 材料科学 · 物理化学 · 辐射探测技术
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Advanced Materials Technologies · 2025 · IF 6.2

Enhanced Detection and Stability Performance of Single-Crystal Perovskite Detectors via Solvent-Based Surface Treatments

Maojun Sun,Zuhao Li,Lu Liang,Tong Chen,Qiang Lou,Lin Zhao,Jiazheng Wang,Xinxin Xu,Bosen Zhang,Yufeng Jin,Hang Zhou

Solution-grown metal halide perovskite single crystals (MHP SCs) hold significant promise for applications in photodetection and high-energy radiation detection. However, the detection performance and long-term operational durability of single-crystal perovskite detectors are hindered by surface defects. Conventional mechanical grinding and polishing methods are time-consuming and labor-intensive, and inevitably pose potential risks related to environmental pollution. In this work, a multiple solvent-based surface engineering strategy is proposed to mitigate these issues. By utilizing the 1-octadecene buffer layer and 1-ethyl-3-methylimidazolium bromide (EMIMBr) ionic liquid passivation agent, the surface morphology is effectively improved and the surface defects of MAPbBr 3 single crystals (MPB SCs) are passivated. The treated MPB SCs demonstrate a substantial increase in photoluminescence intensity, nearly five times greater than that of the untreated samples, along with a prolonged PL lifetime. The photodetectors based on treated MPB SCs exhibit a suppressed dark current of 13.5 nA at a bias of 1 V, and improved response speed. Notably, after 110 days, the unencapsulated devices maintain reliable photodetection performance. Benefiting from suppressed leakage current noise, the planar radiation detectors with an Au/MPB SCs/Au device structure exhibit distinct response to 241 Am@5.49 MeV alpha particles at room temperature.

研究领域: 材料科学 · 光电检测 · 表面工程
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ACS Photonics · 2025 · IF 6.7

Suppression of Secondary Phases with Additive Engineering for the Spectrometer-Grade CsPbBr3 Single Crystals

Yongning Liu,Minghao Cui,Xiaoxi Feng,Wenzhen Wang,Xudong Tang,Sirui Bao,Kunpeng Mou,Benlan Zeng,Fangxiong Tang,Jianing Hu,Huaxing Gou,Jinkun Liu,Yan Zhu,Run Xu

CsPbBr3 single crystals have garnered significant attention as one of the most promising candidates for room-temperature semiconductor radiation detectors. However, the current solution-based growth of CsPbBr3 single crystals suffers from issues of the formation of secondary phases (CsPb2Br5) and strain-induced cracks in crystals due to high growth temperatures above the phase transition. In this study, 4-bromobutyric acid (BBA) as an additive was introduced in the precursor, which leads to an effective suppression of secondary phase formation and simultaneously a reduction of the crystal growth temperature. The CsPbBr3 single crystals grown with BBA exhibited improved crystal quality, with a full width at half-maximum of (200) X-ray rocking curve (XRC) as low as 0.025° and a high hole mobility-lifetime product (μτh) of 0.57 × 10–4 cm2/V. Moreover, the energy resolution for 57Co γ-ray spectra was improved to around 15.2%, indicating a great improvement in transport properties for CsPbBr3 single crystals grown with BBA. This study suggests that the effective suppression of the CsPb2Br5 secondary phase is likely one of the most important issues for a spectrometer-grade CsPbBr3 detector.

研究领域: 材料科学 · 辐射探测技术
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Journal of Materials Chemistry A · 2020 ·Vol. 8 ·期 10 ·5217-5226 · IF 11.301

Purely organic 4HCB single crystals exhibiting high hole mobility for direct detection of ultralow-dose X-radiation

Dou Zhao,Meng Xu,Bao Xiao,Binbin Zhang,Lei Yan,Guoqiang Zeng,Alain Dubois,Paul Sellin,Wanqi Jie,Yadong Xu

Precise detection of low-dose X-radiation using purely organic direct detectors is vital for tissue-equivalent dosimeters and safety control in medical radiation treatment, but it still remains a challenge. Here, we report a promising organic radiation detector based on 4-hydroxycyanobenzene (4HCB, C7H5NO) single crystals. Plate-like 4HCB single crystals up to 18 × 15 × 1.2 mm3 in size are obtained by an optimized solvent evaporation method, thanks to the clarification of the two-dimensional nucleation growth mechanism. After post surface treatment, the leakage current of the 4HCB detector is no larger than 0.1 pA under an electric field of 600 V cm−1. The fabricated detectors show a capability of detecting 241Am 5.49 MeV α particles with a well resolved full energy peak. The calculated hole mobility (μh) and hole mobility lifetime product (μτ)h are 3.40 cm2 V−1 s−1 and 8.50 × 10−5 cm2 V−1, respectively. Simultaneously, under a 50 kVp X-ray beam, a detection limit as low as 0.29 μGyair s−1 with a high sensitivity of 10 μC Gyair−1 cm−2 is achieved in the bias range of 40–100 V, contributing to a superior X-ray imaging capability with a spatial resolution of 0.9 lp mm−1 at a low-dose rate (below 150 μGyair s−1) of exposure.

研究领域: 材料科学 · 医学物理 · 辐射探测技术
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ACS Applied Materials & Interfaces · 2021 · IF 9.229

Solution-Grown Formamidinium Hybrid Perovskite (FAPbBr3) Single Crystals for α-Particle and γ-Ray Detection at Room Temperature

Xin Liu,Meng Xu,Yingying Hao,Jinghua Fu,Fangbao Wang,Binbin Zhang,Stephanie Bennett,Paul Sellin,Wanqi Jie,Yadong Xu

Compared with the widely reported MAPbBr3 single crystals, formamidinium-based (FA-based) hybrid perovskites FAPbBr3 (FPB) with superior chemical and structure stability are expected to be more efficient and perform as more reliable radiation detectors at room temperature. Here, we employ an improved inverse temperature crystallization method to grow FPB bulk single crystals, where issues associated with the retrograde solubility behavior are resolved. A crystal growth phase diagram has been proposed, and accordingly, growth parameters are optimized to avoid the formation of NH4Pb2Br5 secondary phase. The resulting FPB crystals exhibit a high resistivity of 2.8 × 109 Ω·cm and high electron and hole mobility–lifetime products (μτ) of 8.0 × 10–4 and 1.1 × 10–3 cm2·V–1, respectively. Simultaneously, the electron and hole mobilities (μ) are evaluated to be 22.2 and 66.1 cm2·V–1·s–1, respectively, based on the time-of-flight technique. Furthermore, a Au/FPB SC/Au detector is constructed that demonstrates a resolvable gamma peak from 59.5 keV 241Am γ-rays at room temperature for the first time. An energy resolution of 40.1% is obtained at 30 V by collecting the hole signals. These results demonstrate the great potential of FAPbBr3 as a hybrid material for γ-ray spectroscopy and imaging.

研究领域: 材料科学 · 物理学
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JOURNAL OF MATERIALS SCIENCE & TECHNOLOGY · 2025 · IF 14.3

Controlled high-quality perovskite single crystals growth for radiation detection: Nucleation and growth kinetics of antisolvent vapor-assisted crystallization

Jiayi Li,Yazhou Yang,Zhenglan Ye,Dan Chen,Jinlai Cui,Qinxing Huang,Yupeng Zhu,Guangze Zhang,Tao Men,Yuhua Zuo,Jun Zheng,Lei Zhao,Chunlan Zhou,Zhi Liu,Buwen Cheng

Perovskite single crystals (PSCs) have attracted significant interest for next-generation radiation detection. However, the lack of in-depth crystal growth kinetics of PSCs limits the development of high-quality PSCs. Here, with an in-situ real-time monitoring system for MAPbBr 3 PSCs growth during the antisolvent vapor-assisted crystallization (AVC) process, the growth curves of MAPbBr 3 PSCs are obtained and the growth kinetics are theoretically modeled. Two important factors, including antisolvent vapor flux and initial precursor concentration, have been investigated experimentally for their impacts on crystal quality. By controlling the antisolvent vapor flux, the nucleation of PSCs at the container-solution interface can be regulated; while by controlling the initial precursor concentration, the crystal quality can be improved. The optimized MAPbBr 3 PSCs exhibited significantly high qualities, with the narrowest reported full width at half maximum (0.00637°) of X-ray diffraction rocking curve as reported, a trap-state density as low as 2.12 × 10 10 cm −3 , and a mobility-lifetime ( μτ ) product of 1.4 × 10 −2 cm 2 V −1 . The fabricated X-ray detectors demonstrated optimal performance at an electric field of 20 V/mm, with a sensitivity of 9.02 × 10 3 μC Gy −1 cm −2 and the lowest detectable dose rate of 0.08 μGy s −1 under irradiation with continuum X-ray energy up to 20 keV. This work provides valuable insights for the development of high-quality PSCs for direct radiation detection.

研究领域: 材料科学 · 物理学 · 辐射探测技术
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Science China-Chemistry · 2018 ·Vol. 61 ·期 12 ·1581-1586 · IF 4.448

X-ray scintillation in lead-free double perovskite crystals

Hu Qingsong,Deng Zhenzhou,Hu Manchen,Zhao Anjiang,Zhang Yaqi,Tan Zhifang,Niu Guangda,Wu Haodi,Tang Jiang

Metal halide perovskites have shown great performance for various applications, including solar cells, light emitting diodes, and radiation detectors, but they still suffer from the toxicity of lead and instability. Here we report the use of lanthanide series as trivalent metals to obtain low toxicity and highly stable double perovskites (Cs 2 NaLnCl 6 , Ln=Tb or Eu) with high scintillation light yield. The crystals exhibit typical f-f transitions of lanthanide cations, while Cs 2 NaTbCl 6 exhibits strong green photoluminescence, and Cs 2 NaEuCl 6 exhibits red photoluminescence. Under X-ray radiations, the light yield of Cs 2 NaTbCl 6 reaches 46600 photons MeV −1 , much higher than that of the commercially used (Lu,Y) 2 SiO 5 :Ce 3+ crystals (LYSO, 28500 photons MeV −1 ), and previously reported lead-based perovskites (14000 photons MeV −1 ). As a new member of lead-free perovskites, lanthanide-based double perovskites open up a new route toward radiation detections and potential medical imaging.

CAS / MDL: 7647-17-8
研究领域: 材料科学 · 辐射物理 · 光学材料 · 医学成像
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