Abstract

Continuously growing evidence of the excellent radiation hardness of perovskite solar cells stimulates their intense exploration in the context of potential aerospace applications. However, there is still a very limited understanding of the fundamental aspects such as the mechanisms of the interaction of complex lead halides with different types of ionizing radiation and associated aging pathways, even though this knowledge is essentially important for the development of new materials with improved properties. Herein, we made one of the first steps to fill this gap through a systematic study of the aging behavior of two perovskite absorber materials under exposure to three different stressors: 60Co gamma-rays, 8.5 MeV electron fluences, and light. The application of a set of complementary spectroscopy and microscopy techniques allowed us to identify and compare perovskite degradation pathways caused by each type of the ionizing radiation. In particular, radiation-induced phase segregation with the formation of δ-phases of CsPbI3 and FAPbI3 appears to be a common route in the case of double cation perovskites. Most importantly, we have revealed that the incorporation of dysprosium cations as a replacement of 1 % of Pb2+ ions in the Cs0.12FA0.88Pb0.99Dy0.01I3 material formulation results in a remarkably improved radiation hardness: this modification blocks the formation of metallic lead and strongly suppresses segregation of Cs-rich and FA-rich phases in perovskite films under exposure to gamma rays or high-energy electrons. Thus, these results open up a promising research direction for designing radiation-resistant perovskite absorbers through rational compositional engineering.

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