Perovskite detectors for x-ray imaging and gamma spectroscopy: overview and current state-of-the-art

Perovskites are a family of semiconductor materials with molecular formula ABX3 [where A+ = Cesium (Cs), methylammonium (MA or CH3NH3) or formamidinium (FA or CH(NH2)2), B-site is metal, and X− = chlorine (Cl), bromine (Br) or iodine (I)] that have recently seen a surged interest for X-ray and gamma-ray detection. The all inorganic version, CsPbBr3, grown by high temperature melt method has been demonstrated with an impressive gamma-ray energy resolution of 1.4%@662 keV, while the solution grown CsPbBr3 showed the best achievable resolution of 5.5% at the same energy from a 137Cs source. This paper gives an overview of the development of perovskite in both X-ray detection and gamma spectroscopy, including the most recent advancement with perovskite single crystal grown by low temperature inverse temperature method for solid-state X-ray detector. The crystal shows a decent long carrier diffusion length that is ideal for charge collection, while their mobilities are still not on par with CdZnTe. We also reported our most recent development on clarifying the concepts around X-ray detection limits. The X-ray sensitivity and the lowest detectable dose rate (i.e., X-ray detection limits) of several MAPbI3 detectors made of single crystal were experimentally measured. The best achieved X-ray sensitivity is ~2.5E4 μC/Gyair/cm2 under 15.4 V/mm, which is comparable to the current state-of-the-art MAPbI3 based X-ray detectors (~ 2.3E4 μC/Gyair/cm2 under 4.2 V/mm for GAMAPbI3 (GA=guanidinium) single crystal detector). The best achieved lowest detectable X-ray dose rate for the same MAPbI3 detector is ~61 nGyair/s under 15.4 V/mm, and decreased to ~24 nGyair/s under 3.8 V/mm. The good performance of the MAPbI3 detectors further proves their great potential as the next generation low-cost X-ray detector.

[1]  X. Ren,et al.  Thinness‐ and Shape‐Controlled Growth for Ultrathin Single‐Crystalline Perovskite Wafers for Mass Production of Superior Photoelectronic Devices , 2016, Advanced materials.

[2]  Safa Kasap,et al.  Amorphous selenium as an X-ray photoconductor , 2004 .

[3]  Thilo Michel,et al.  High-performance direct conversion X-ray detectors based on sintered hybrid lead triiodide perovskite wafers , 2017, Nature Photonics.

[4]  Guangda Niu,et al.  Rubidium Doping to Enhance Carrier Transport in CsPbBr3 Single Crystals for High-Performance X-Ray Detection. , 2019, ACS applied materials & interfaces.

[5]  Kanai S. Shah,et al.  Mercuric iodide and lead iodide x-ray detectors for radiographic and fluoroscopic medical imaging , 2003, SPIE Medical Imaging.

[6]  Habib Mani,et al.  Amorphous and Polycrystalline Photoconductors for Direct Conversion Flat Panel X-Ray Image Sensors , 2011, Sensors.

[7]  Yang Yang,et al.  Perovskite semiconductors for direct X-ray detection and imaging , 2020, Journal of Semiconductors.

[8]  M. Kanatzidis,et al.  Zero-Dimensional Cs2TeI6 Perovskite: Solution-Processed Thick Films with High X-ray Sensitivity , 2019, ACS Photonics.

[9]  Alain Goriely,et al.  High-quality bulk hybrid perovskite single crystals within minutes by inverse temperature crystallization , 2015, Nature Communications.

[10]  Safa Kasap,et al.  Springer Handbook of Electronic and Photonic Materials , 2007 .

[11]  Yanbin Chen,et al.  High Performance X-ray Detection Based on One-Dimensional Inorganic Halide Perovskite CsPbI3. , 2019, The journal of physical chemistry letters.

[12]  L. A. Currie,et al.  LIMITS FOR QUALITATIVE DETECTION AND QUANTITATIVE DETERMINATION. APPLICATION TO RADIOCHEMISTRY. , 1968 .

[13]  M. Kanatzidis,et al.  CsPbBr3 perovskite detectors with 1.4% energy resolution for high-energy γ-rays , 2021 .

[14]  Jinsong Huang,et al.  Monolithic integration of hybrid perovskite single crystals with heterogenous substrate for highly sensitive X-ray imaging , 2017, Nature Photonics.

[15]  M. Kanatzidis,et al.  Nucleation-controlled growth of superior lead-free perovskite Cs3Bi2I9 single-crystals for high-performance X-ray detection , 2020, Nature Communications.

[16]  K. Lynn,et al.  Effects of excess Te on flux inclusion formation in the growth of cadmium zinc telluride when forced melt convection is applied , 2020 .

[17]  X. Miao,et al.  Hot‐Pressed CsPbBr3 Quasi‐Monocrystalline Film for Sensitive Direct X‐ray Detection , 2019, Advanced materials.

[18]  Tim B F Woodfield,et al.  First human imaging with MARS photon-counting CT , 2018, 2018 IEEE Nuclear Science Symposium and Medical Imaging Conference Proceedings (NSS/MIC).

[19]  Jinsong Huang,et al.  Comparison of Zr, Bi, Ti, and Ga as Metal Contacts in Inorganic Perovskite CsPbBr₃ Gamma-Ray Detector , 2020, IEEE Transactions on Nuclear Science.

[20]  Sang Yoon Lee,et al.  Printable organometallic perovskite enables large-area, low-dose X-ray imaging , 2017, Nature.

[21]  Don Ouimette A new large area x-ray image sensor , 1997 .

[22]  E. Kymakis,et al.  Metal Halide Perovskites for High‐Energy Radiation Detection , 2020, Advanced science.

[23]  M. Kanatzidis,et al.  Perovskite CsPbBr3 single crystal detector for alpha-particle spectroscopy , 2019, Nuclear Instruments and Methods in Physics Research Section A: Accelerators, Spectrometers, Detectors and Associated Equipment.

[24]  M. Kanatzidis,et al.  Resolving the Energy of γ-Ray Photons with MAPbI3 Single Crystals , 2018, ACS Photonics.

[25]  E. Sargent,et al.  Low trap-state density and long carrier diffusion in organolead trihalide perovskite single crystals , 2015, Science.

[26]  M. Kanatzidis,et al.  High-sensitivity X-ray detectors based on solution-grown caesium lead bromide single crystals , 2020 .

[27]  M. Z. Kabir Effects of charge carrier trapping on polycrystalline PbO x-ray imaging detectors , 2008 .

[28]  Haiming Zhu,et al.  Highly sensitive X-ray detector made of layered perovskite-like (NH4)3Bi2I9 single crystal with anisotropic response , 2019, Nature Photonics.

[29]  Jinsong Huang,et al.  Dopant compensation in alloyed CH3NH3PbBr3-xClx perovskite single crystals for gamma-ray spectroscopy. , 2017, Nature materials.

[30]  Qingfeng Dong,et al.  Electron-hole diffusion lengths > 175 μm in solution-grown CH3NH3PbI3 single crystals , 2015, Science.

[31]  Martin Hoheisel,et al.  Review of medical imaging with emphasis on X-ray detectors , 2006 .

[32]  Zhifu Liu,et al.  Crystal Growth of the Perovskite Semiconductor CsPbBr3: A New Material for High-Energy Radiation Detection , 2013 .

[33]  A. Strasheim,et al.  NOMENCLATURE, SYMBOLS, UNITS AND THEIR USAGE IN , 1985 .

[34]  Haotong Wei,et al.  Halide lead perovskites for ionizing radiation detection , 2019, Nature Communications.

[35]  Jinsong Huang,et al.  Scalable fabrication of efficient organolead trihalide perovskite solar cells with doctor-bladed active layers , 2015 .

[36]  Yemin Dong,et al.  Flexible, Printable Soft‐X‐Ray Detectors Based on All‐Inorganic Perovskite Quantum Dots , 2019, Advanced materials.

[37]  Jinsong Huang,et al.  Low defects density CsPbBr3 single crystals grown by an additive assisted method for gamma-ray detection , 2020, Journal of Materials Chemistry C.

[38]  Jinsong Huang,et al.  Ligand assisted growth of perovskite single crystals with low defect density , 2021, Nature Communications.

[39]  Jun Chen,et al.  A-site Cation Engineering for Highly Efficient MAPbI3 Single Crystal X-ray Detector. , 2019, Angewandte Chemie.

[40]  Safa Kasap,et al.  Photoconductors for X-Ray Image Detectors , 2017 .

[41]  Guangda Niu,et al.  Cs2AgBiBr6 single-crystal X-ray detectors with a low detection limit , 2017 .

[42]  Wei Zhao,et al.  Robust Fabrication of Hybrid Lead‐Free Perovskite Pellets for Stable X‐ray Detectors with Low Detection Limit , 2020, Advanced materials.

[43]  Jinsong Huang,et al.  Perovskite-filled membranes for flexible and large-area direct-conversion X-ray detector arrays , 2020 .

[44]  Philipp Lodomez,et al.  Characterization of charge collection in CdTe and CZT using the transient current technique , 2006 .

[45]  X. Miao,et al.  Unveiling the Structural Descriptor of A3B2X9 Perovskite Derivatives toward X‐Ray Detectors with Low Detection Limit and High Stability , 2020, Advanced Functional Materials.

[46]  Padhraic Mulligan,et al.  Sensitive X-ray detectors made of methylammonium lead tribromide perovskite single crystals , 2016, Nature Photonics.

[47]  Safa Kasap,et al.  X-ray sensitivity of photoconductors: application to stabilized a-Se , 2000 .

[48]  K. Zhao,et al.  Large and Dense Organic-Inorganic Hybrid Perovskite CH3NH3PbI3 Wafer Fabricated by One-Step Reactive Direct Wafer Production with High X-ray Sensitivity. , 2020, ACS applied materials & interfaces.

[49]  Sergei Tretiak,et al.  High-efficiency solution-processed perovskite solar cells with millimeter-scale grains , 2015, Science.

[50]  Jinsong Huang,et al.  Performance of Perovskite CsPbBr3 Single Crystal Detector for Gamma-Ray Detection , 2020, IEEE Transactions on Nuclear Science.