Proceedings of International Conference on Hybrid and Organic Photovoltaics (HOPV24)
DOI: https://doi.org/10.29363/nanoge.hopv.2024.253
Publication date: 6th February 2024
Metal-halide perovskites require careful growth and defect passivation strategies to reach the highest efficiency and exhibit improved long-term operational stability in optoelectronic devices. Non-radiative defect-mediated charge-carrier recombination can be inhibited by modifying perovskites with molecular compounds as passivating agents. Recently, silanes, a new generation of passivating agents, have been shown to work excellently, not only passivating the modified surface sites but also providing a hydrophobic layer giving moisture protection. Our collaborators have shown amino-silane treated FAPbI3 based perovskite solar cells to maintain 95 per cent of their initial efficiency for more than 1,600 hours when subjected to full-spectrum simulated sunlight at 85 ℃, under open-circuit conditions in ambient air. However, the structures and interactions of these silane molecules at the perovskite surfaces are not fully understood at the atomic level. Our density functional theory and ab initio molecular dynamics simulations reveal atomic-scale details of strong passivator binding of the amino-silane molecules on the defective perovskite surface. Changes in the charge density profile around all the species show silane-surface charge transfer around the surface Pb cations. Since the surface Pb ions adjacent to iodide vacancies are severely undercoordinated, the amino-silane adsorption through both N-Pb and O-Pb bonds acts by increasing the Pb coordination and eliminating the effects of surface vacancy defects, thereby effectively passivating the perovskite surface. Overall, these ab-initio simulation results also agree with our experimental findings and provide new structural and mechanistic insights at the atomic level.