Proceedings of MATSUS Spring 2025 Conference (MATSUSSpring25)
DOI: https://doi.org/10.29363/nanoge.matsusspring.2025.133
Publication date: 16th December 2024
Metal Halide Perovskites (MHPs) and their derivatives are the subject of intense research due to their remarkable optoelectronic properties and tunable bandgap [1]. Major applications include photovoltaic cells for three-dimensional perovskites, as well as photodetectors, photodiodes, and lasers for other perovskite-based materials. A significant modification that can be made to organic-inorganic metal halides is the introduction of chiral organic cations, leading to the emergence of chiroptical properties and the Rashba-Edelstein effect [2]. The latter is particularly interesting for spin-related phenomena such as chirality-induced spin selectivity (CISS).To date, most chiral metal halides contain lead, a toxic element subject to strict regulations. Therefore, the exploration of lead-free materials is crucial. In this study, we report the synthesis of bismuth (III)- and antimony (III)-containing chiral iodides, including R/S-1-(4-Chloro)-Phenylethylammonium (abbreviated as Cl-PEA) as the organic chiral cation. Single crystals with the stoichiometry Cl-PEA₄M₂I₁₀ (where M represents Bi or Sb) have been prepared for both enantiomers and the racemic compound, and their structures have been resolved via single-crystal XRD. Additionally, mixed Sb/Bi systems have been synthesized to investigate potential bandgap bowing, which has already been observed in analogous vacancy-ordered achiral perovskites [3], and already analysed via powder diffraction.The optical properties of the prepared samples have been analyzed using UV-Vis and CD spectroscopy. Finally, starting from the experimental data, computational modeling has been employed to optimize the crystal structures, determine the electronic band structure, and evaluate the presence and extent of Rashba splitting. The modeling has also been used to calculate the projected density of states (PDOS) and the total density of states (DOS) of our compounds. These calculations provide insights into the orbital contributions to the observed bandgap bowing and identify the contributing species.
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