Proceedings of MATSUS Spring 2024 Conference (MATSUS24)
DOI: https://doi.org/10.29363/nanoge.matsus.2024.048
Publication date: 18th December 2023
Inter alia, the application of 2D phenylethylammonium lead quaternary iodide (PEA2PbI4)/three-dimensional (3D) metal halide perovskite (MHP) interfaces has improved various optoelectronic devices, where a staggered type-II energy level alignment was often assumed. However, a type-II heterojunction seems to contradict the enhanced photoluminescence observed for 2D PEA2PbI4/3D MHP interfaces, which raises fundamental questions about the electronic properties of such junctions. Using direct and inverse photoelectron spectroscopy, we reveal that a straddling type-I energy level alignment is present at 2D PEA2PbI4/3D methylammonium lead triiodide (MAPbI3) interfaces, thus explaining that the photoluminescence enhancement of the 3D perovskite is induced by energy transfer from the 2D perovskite.
On another note, formamidinium lead triiodide (FAPbI3) is gaining attention as a perovskite solar absorber due to its close to optimal bandgap for single-junction solar cells and enhanced thermal stability compared to many other MHPs. However, in order to achieve the stable black-phase FAPbI3, a relatively high temperature annealing (150 °C) is required. Recent studies have highlighted the impact of high-temperature annealing on FAPbI3 crystal structure originating from lattice distortion and volume expansion. Nonetheless, the fundamental understanding of its electronic properties remained unclear. Here, we show that intrinsic iodine vacancies lead to n-type character, and that in-diffusing oxygen can fill iodine vacancies, leading to a Fermi level shift towards the valence band by about 0.5 eV. Furthermore, we demonstrate how the energy levels at interface to charge selective contacts can be controlled by doping, and how this influences the quasi-Fermi level splitting under illumination due to charge accumulation at the interface.
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