Investigation of Two‐Dimensional Ruddlesden–Popper BZA2PbX4 (X = I, Br, and Cl) and Mixed‐Halides BZA2PbBrxCl4−x Perovskites: Opto‐Electromechanical, Thermodynamic Properties, Moisture, and Strain Effects

Abstract

Herein, the properties of BZA2PbX4 (X = I, Br, and Cl) and mixed halides BZA2PbBrxCl4‐x (x = 1, 2, and 3) perovskites are comprehensively investigated, utilizing density functional theory (DFT). As there has been no prior comprehensive study on the substantial characteristics of mixed halides and the distinctive features of BZA2PbI4, BZA2PbBr4, and BZA2PbCl4 using DFT, a significant gap in the existing literature is addressed. The optical and electronic properties, band structures, band edge orbitals, and effective masses with and without spin‐orbit coupling effects are analyzed. The investigation also examines the impact of strain (tensile and compressive) on the properties of these materials. It is revealed that among the investigated compounds, BZA2PbCl4 emerges as the most thermodynamic and moisture stable. This trend is corroborated by the energy fluctuation, with BZA2PbCl4 demonstrating a narrower range, indicative of superior thermal stability. Furthermore, Voigt–Ruess–Hill approximations indicate that the mechanical moduli increase as the halide changes from I to Cl. Moreover, BZA2PbI4 exhibits the highest level of disorder, whereas BZA2PbCl4 has the lowest entropy value at the same temperature. The results highlight that these materials emerge as promising candidates for applications in the active layer of perovskite light‐emitting diodes and optoelectronic devices.