Abstract
Lead halide perovskites have become a leading material in the field of emerging photovoltaics and optoelectronics. Significant progress has been achieved in improving the intrinsic properties and environmental stability of these materials. However, the stability of lead halide perovskites to ionising radiation has not been widely investigated. In this study, we investigated the radiolysis of lead halide perovskites with organic and inorganic cations under X-ray irradiation using synchrotron based hard X-ray photoelectron spectroscopy. We found that fully inorganic perovskites are significantly more stable than those containing organic cations. In general, the degradation occurs through two different, but not mutually exclusive, pathways/mechanisms. One pathway is induced by radiolysis of the lead halide cage into halide salts, halogen gas and metallic lead and appears to be catalysed by defects in the perovskite. The other pathway is induced by the radiolysis of the organic cation which leads to formation of organic degradation products and the collapse of the perovskite structure. In the case of Cs0.17FA0.83PbI3, these reactions result in products with a lead to halide ratio of 1 : 2 and no formation of metallic lead. The radiolysis of the organic cation was shown to be a first order reaction with regards to the FA+ concentration and proportional to the X-ray flux density with a radiolysis rate constant of 1.6 × 10-18 cm2 per photon at 3 keV or 3.3 cm2 mJ-1. These results provide valuable insight for the use of lead halide perovskite based devices in high radiation environments, such as in space environments and X-ray detectors, as well as for investigations of lead halide perovskites using X-ray based techniques.
Highlights
IntroductionThe stability to ionising radiation becomes one of the most important factors
For certain applications, the stability to ionising radiation becomes one of the most important factors
We have investigated the X-ray stability of lead halide perovskites with a particular focus on two different, relatively stable, perovskite compositions
Summary
The stability to ionising radiation becomes one of the most important factors One such application is the deployment of solar cells for powering spacecrafts where the requirements are quite different from terrestrial deployment. Most significant being the lack of atmosphere (and no moisture or oxygen), extreme temperature variations, and significantly higher exposure to ionizing radiation. Another example is the usage as radiation detectors, where early studies indicate that the performance of wide bandgap lead halide perovskites is competitive to currently used materials,[7] and with the additional benefit that they can be deposited on flexible substrates.[8] The most promising candidates for this kind of applications appear to be MAPbBr39,10 and CsPbBr3.11–13.
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