Properties of PeDAPbI4 Dion-Jacobson phase perovskite regulated by ligand with amino and hydroxy

Dion-Jacobson (DJ) phase perovskites have garnered considerable attention due to their potential for enhancing the stability of optoelectronic devices. In this paper, the electronic, structural, and optical properties of 16 NH₃(CH₂)₅NH₃PbI₄ (PeDAPbI₄) models (9 amino models (AM) and 7 hydroxyl models (HM)) based on different positions of amino and hydroxyl groups are investigated. Among the AM, the binding energy (E_c) ranges from −136.768 eV to −137.950 eV. The value of bandgap (E_g) ranges from 2.052 eV to 2.865 eV. In the HM, the E_c ranges from −143.330 eV to −144.367 eV. The value of E_g varies from 2.103 eV to 2.870 eV, which is approximately consistent with the bandgap variation range of the AM. The optical properties reveal that the light absorption of the AM primarily depends on the symmetry of the amino groups in the ligand, with lower symmetry leading to stronger absorption, while the hydroxyl group also exerts a certain impact. According to our results, both amino and hydroxyl groups regulate the bandgap, and hydroxyl groups further enhance the stability, giving DJ phase perovskites significant potential for application in optoelectronic devices.