Proceedings of MATSUS Spring 2024 Conference (MATSUS24)
DOI: https://doi.org/10.29363/nanoge.matsus.2024.278
Publication date: 18th December 2023
Metal halide perovskites emerged as outstanding materials for optoelectronics due to their excellent optoelectronic properties, such as direct and tunable band gaps, large absorption cross sections and long lifetimes and diffusion paths of the charge carriers.[1] So far, the field has been dominated by lead-based perovskites, but issues concerning lead toxicity and stability have led to explore new possible perovskite candidates. In this context tin and double perovskites of different dimensionalities have attracted increasing interest.[2,3] The optoelectronic features, as well as the efficiencies of these materials in optoelectronic devices, is largely influenced by the nature of the chemical bond, the defects activity and the coupling of photogenerated charges with the lattice.
In this presentation a theoretical perspective is provided about the influence of chemical composition and dimensionality on the defect activity and the charge carrier photophysics in perovskites beyond the APbX3 composition, by focusing on less-toxic Sn and Bi/Ag double perovskites. The defect chemistry and photophysics of tin and double perovskites will be discussed, by keeping a parallelism between 3D and 2D, i.e. MASnI3 vs PEA2SnI4 and Cs2AgBiBr6 vs (BA)4AgBiBr8 phases, as test cases.[4,5] The analysis aims to highlight the effects of chemical composition and quantum confinement (QC) on several key properties of these materials. The origin of the self p-doping, strongly limiting the efficiency of tin perovskites, will be discussed, as well as computationally designed doping strategies aimed to reduce it. Hence, discussion will move to analyze the charge carrier photophysics in tin and double perovskites, by focusing on the processes possibly originating the sub-gap emissive features in these materials. Specifically, the competition between the exciton self-trapping and trapping/emission at defect centers vs the chemical composition will be discussed.
This contribution aims to provide a theoretical framework guiding experimentalists in the design of stable and efficient lead-free perovskite materials.
This work has received funding from the European Union’s Horizon Europe research and innovation program under grant agreement no. 101082176 - VALHALLA
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