Effect of Chlorine Inclusion in Wide Band Gap FAPbBr₃ Perovskites

Abstract Wide bandgap perovskites have recently gained attention owing to their physical properties, versatility, and potential in various optoelectronic devices including LEDs, detectors, and building‐integrated photovoltaics (BIPV). However, BIPV materials must meet conflicting requirements, necessitating high performance, high transparency in the visible spectrum and color neutrality. This study investigates the controlled addition of chlorine in FAPb(Br_1‐xCl_x)₃ perovskites to achieve band gaps exceeding 2.4 eV. Increasing chlorine content from x_Cl = 0.00 to x_Cl = 0.25 widens the band gap from 2.37 to 2.52 eV, effectively improving the visible light transparency. Advanced characterization techniques including X‐ray diffraction, synchrotron radiation photoelectron spectroscopy, photoluminescence imaging, and fast transient absorption spectroscopy, complemented by density functional theory, reveal insights into absorption properties, electronic structure, and ultrafast recombination dynamics as a function of the thin film chemical composition. Furthermore, this study evaluates energetic disorder, carrier recombination rates, and non‐radiative losses for different compositions by extracting quantitative parameters such as Urbach energy and quasi‐Fermi level splitting, offering novel insights and guidelines for the design and optimization of emerging photovoltaic (PV) materials. Optimal PV performance metrics are achieved with a wide bandgap bromine perovskite containing 14% chlorine, striking a balance between morphology, transparency, and voltage losses.