Proceedings of MATSUS Fall 2023 Conference (MATSUSFall23)
DOI: https://doi.org/10.29363/nanoge.matsus.2023.140
Publication date: 18th July 2023
Tin-lead (Sn-Pb) halide perovskites stand out as top candidates for future near-infrared (NIR) optoelectronics, being particularly promising in all-perovskite tandem solar cells and NIR photodetectors. However, their facile degradation under operational conditions (e.g., ambient-mediated oxidation of Sn2+) remains the main impediment towards their widespread deployment. To enable the design of Sn-Pb perovskite compositions with higher innate stability, it is critical to unravel how the constituent ions of perovskite besides Sn2+ participate in the degradation of these materials. Specifically, the inconspicuous role of A-site cations in the decomposition of technologically relevant ASn0.5Pb0.5I3 perovskite structures has been largely overlooked.
In this talk, I will describe the effect that A-site cation tuning has on the degradation mechanism under ambient air of Sn-Pb perovskite compositions commonly employed in solar cells, i.e., CsxMA0.3-xFA0.7Sn0.5Pb0.5I3 (where x = 0, 0.15 and 0.3; MA = methylammnonium; FA = formamidinium). By employing thermogravimetric and spectroscopic techniques, we track the formation of molecular iodine (I2) and tin(IV) iodide (SnI4) versus time as indicators of perovskite degradation caused by exogenous O2 and endogenous I2, respectively. We detect the rate of I2 and SnI4 generation to be approximately one order of magnitude lower for Cs-rich compositions relative to their MA-rich counterparts, clearly indicating that MA replacement by Cs leads to enhanced resilience against oxidative stress. Consequently, this translates into higher stability of optical, electrical and structural properties in Cs-rich perovskite thin films upon air exposure. The talk will conclude with details on the origin of the lower stability of MA-rich compositions, which we ascribe to stronger I2 adsorption at the surface of perovskite mediated by the polarising power of the MA cation. This work provides key insights on the role of A-site choice on perovskite degradation that serve as valuable guidelines for the design of Sn-Pb perovskite optoelectronics with enhanced stability.
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