The effective detection of X-ray radiation with low threshold is essential to many medical and industrial applications. Three-dimensional (3D) organolead trihalide and double perovskites have been shown to be suitable for direct X-ray detection. However, the sensitivity and stability of 3D perovskite X-ray detectors are limited by ion motion, and there remains a demand to develop green and stable X-ray detectors with high sensitivity and low detection limit. The emerging low-dimensional perovskites have shown promising optoelectronic properties, featuring good intrinsic stability and reduced ion migration. Inspired by this, we show that our 2D layered perovskite-like (NH4)3Bi2I9 device provides unique anisotropic X-ray detecting performance with different crystal directions, effective suppression of ion migration and a low detection limit of 55 nGyair s−1. These results will motivate new strategies to achieve a high-performance X-ray detector by utilizing 2D layered perovskite or perovskite-like materials, without requiring toxic elements.
Subscribe to Journal
Get full journal access for 1 year
only $15.58 per issue
All prices are NET prices.
VAT will be added later in the checkout.
Rent or Buy article
Get time limited or full article access on ReadCube.
All prices are NET prices.
The data that support the plots within this paper and other findings of this study are available from the corresponding author on reasonable request.
Jiang, Q. et al. Surface passivation of perovskite film for efficient solar cells. Nat. Photon. https://doi.org/10.1038/s41566-019-0398-2 (2019).
Brenner, T. M., Egger, D. A., Kronik, L. K., Hoder, G. H. & Cahen, D. Hybrid organic–inorganic perovskites: low-cost semiconductors with intriguing charge-transport properties. Nat. Rev. Mater. 1, 15007 (2016).
Heiss, W. & Brabec, C. X-ray imaging: perovskites target X-ray detection. Nat. Photon. 10, 288–289 (2016).
Jeong, M., Jo, W. J., Kim, H. S. & Ha, J. H. Radiation hardness characteristics of Si-PIN radiation detectors. Nucl. Instrum. Methods Phys. Res. A 784, 119–123 (2015).
Luke, P. N., Rossington, C. S. & Wesela, M. F. Low energy X-ray response of Ge detectors with amorphous Ge entrance contacts. IEEE Trans. Nucl. Sci. 41, 1074–1079 (1994).
Szeles, C. CdZnTe and CdTe materials for X-ray and gamma ray radiation detector applications. Phys. Status Solidi B 241, 783–790 (2004).
Zhao, W. & Rowlands, J. A. X-ray imaging using amorphous selenium: feasibility of a flat panel self-scanned detector for digital radiology. Med. Phys. 22, 1595–1604 (1995).
Chen, Q. et al. All-inorganic perovskite nanocrystal scintillators. Nature 561, 88–93 (2018).
Heo, J. H. High-performance next-generation perovskite nanocrystal scintillator for nondestructive X-ray imaging. Adv. Mater. 30, 1801743 (2018).
Yakunin, S. et al. Detection of X-ray photons by solution-processed lead halide perovskites. Nat. Photon. 9, 444–449 (2015).
Shrestha, S. et al. High-performance direct conversion X-ray detectors based on sintered hybrid lead triiodide perovskite wafers. Nat. Photon. 11, 436–440 (2017).
Wei, H. et al. Sensitive X-ray detectors made of methylammonium lead tribromide perovskite single crystals. Nat. Photon. 10, 333–339 (2016).
Wei, W. et al. Monolithic integration of hybrid perovskite single crystals with heterogenous substrate for highly sensitive X-ray imaging. Nat. Photon. 11, 315–321 (2017).
Kim, Y. C. et al. Printable organometallic perovskite enables large-area, low-dose X-ray imaging. Nature 550, 87–91 (2017).
Dong, Q. et al. Electron–hole diffusion lengths >175 μm in solution-grown CH3NH3PbI3 single crystals. Science 347, 967–970 (2015).
Shi, D. et al. Low trap-state density and long carrier diffusion in organolead trihalide perovskite single crystals. Science 347, 519–522 (2015).
Saidaminov, M. I. et al. High-quality bulk hybrid perovskite single crystals within minutes by inverse temperature crystallization. Nat. Commun. 6, 7586 (2015).
Lui, Y. et al. A 1300 mm2 ultrahigh-performance digital imaging assembly using high-quality perovskite single crystals. Adv. Mater. 2018, 1707314 (2018).
Mohan, R. Green bismuth. Nat. Chem. 2, 336 (2010).
Pan, W. et al. Cs2AgBiBr6 single-crystal X-ray detectors with a low detection limit. Nat. Photon. 11, 726–732 (2017).
Steele, J. A. et al. Photophysical pathways in highly sensitive Cs2AgBiBr6 double-perovskite single-crystal X-ray detectors. Adv. Mater. 2018, 1804450 (2018).
McCall, K. M. et al. α-Particle detection and charge transport characteristics in the A3M2I9 defect perovskites (A = Cs, Rb; M = Bi, Sb). ACS Photonics 5, 3748–3762 (2018).
Sun, Q. et al. Optical and electronic anisotropies in perovskitoid crystals of Cs3Bi2I9 studies of nuclear radiation detection. J. Mater. Chem. A 6, 23388–23395 (2018).
Sun, S. et al. Synthesis, crystal structure and properties of a perovskite-related bismuth phase, (NH4)3Bi2I9. APL Mater. 4, 031101 (2016).
Xiao, Z., Meng, W., Wang, J., Mitzi, D. B. & Yan, Y. Searching for promising new perovskite-based photovoltaic absorbers: the importance of electronic dimensionality. Mater. Horiz. 4, 206–216 (2017).
Ji, C. et al. Inch-size single crystal of a lead-free organic–inorganic hybrid perovskite for high-performance photodetector. Adv. Funct. Mater. 28, 1705467 (2018).
Evans, R. D. & Noyau, A. The Atomic Nucleus Vol. 582 (McGraw-Hill, 1955).
Abulikemu, M. et al. Optoelectronic and photovoltaic properties of the air-stable organohalide semiconductor (CH3NH3)3Bi2I9. J. Mater. Chem. A 32, 1–24 (2016).
Kawai, T. et al. Optical absorption in band-edge region of (CH3NH3)3Bi2I9 single crystals. J. Phys. Soc. Jpn 65, 1464–1468 (1996).
Ma, Z. et al. Air-stable layered bismuth-based perovskite-like materials: structures and semiconductor properties. Physica B 526, 136–142 (2017).
Correa-Baena, J. P. et al. A-site cation in inorganic A3Sb2I9 perovskite influences structural dimensionality, exciton binding energy, and solar cell performance. Chem. Mater. 30, 3734–3742 (2018).
Lehner, A. J. et al. Crystal and electronic structures of complex bismuth iodides A3Bi2I9 (A = K, Rb, Cs) Related to perovskite: aiding the rational design of photovoltaics. Chem. Mater. 27, 7137–7148 (2015).
Lee, Y. et al. High-performance perovskite–graphene hybrid photodetector. Adv. Mater. 27, 41–46 (2015).
Kim, K. et al. Purification of CdZnTe by electromigration. J. Appl. Phys. 117, 145702 (2015).
Devanathan, R., Corrales, L. R., Gao, F. & Weber, W. J. Signal variance in gamma-ray detectors—a review. Nucl. Instrum. Methods Phys. Res. A 565, 637–649 (2006).
Dvoryankin, V. F. et al. X-ray sensitivity of Cd0.9Zn0.1Te detectors. Tech. Phys. 55, 306–308 (2010).
Kasap, S. O. X-ray sensitivity of photoconductors: application to stabilized a-Se. J. Phys. D 33, 2853–2865 (2000).
Brenner, D. J., Elliston, C. D., Hall, E. J. & Berdon, W. E. Estimated risks of radiationinduced fatal cancer from pediatric CT. Am. J. Roentgenol. 176, 289–296 (2001).
Polischuk, B. T., Shukri, Z., Legros, A. & Rougeot, H. Selenium direct converter structure for static and dynamic X-ray detection in medical imaging applications. Proc. Med. Imag. 1998, 494–504 (1998).
Yun, L. et al. Suppressed ion migration in low-dimensional perovskites. ACS Energy Lett. 2, 1571–1572 (2017).
Shearer, D. R. & Bopaiah, M. Dose rate limitations of integrating survey meters for diagnostic X-ray surveys. Health Phys. 79, S20–S21 (2000).
Clairand, I. et al. Use of active personal dosemeters in interventional radiology and cardiology: tests in laboratory conditions and recommendations—ORAMED project. Radiat. Meas. 46, 1252–1257 (2011).
The authors thank X. Hua and C. Wolverton at Northwestern University for their insightful discussions on the band structure of the perovskite-like materials, and also L. Bai and Y. Su in Zhejiang University for their assistance with material preparations. The authors acknowledge financial support from the National Key Research and Development Program of China (2017YFA0207700), the National Basic Research Program of China (973Program, 2015CB352003), the Outstanding Youth Fund of Zhejiang Natural Science Foundation of China (LR18F050001), the Natural Science Foundation of China (61804134) and the Natural Science Foundation of Fujian Province (2017J01766).
The authors declare no competing interests.
Publisher’s note: Springer Nature remains neutral with regard to jurisdictional claims in published maps and institutional affiliations.
About this article
Cite this article
Zhuang, R., Wang, X., Ma, W. et al. Highly sensitive X-ray detector made of layered perovskite-like (NH4)3Bi2I9 single crystal with anisotropic response. Nat. Photonics 13, 602–608 (2019). https://doi.org/10.1038/s41566-019-0466-7
Rubidium Doping to Enhance Carrier Transport in CsPbBr3 Single Crystals for High-Performance X-Ray Detection
ACS Applied Materials & Interfaces (2020)
A Microchannel‐Confined Crystallization Strategy Enables Blade Coating of Perovskite Single Crystal Arrays for Device Integration
Advanced Materials (2020)
Advanced Functional Materials (2020)
Journal of Materials Chemistry C (2020)
ACS Nano (2020)