Abstract
Lead-tin (Pb-Sn) mixed-halide perovskites show potential for single-junction and tandem solar cells due to their adjustable band gaps, flexible composition, and superior environmental stability compared to three-dimensional (3D) perovskites. However, they have lower power conversion efficiencies. Understanding band alignment and charge carrier dynamics is essential for enhancing photovoltaic performance. In this view, herein we have prepared thin films of mixed Pb-Sn-based two dimensional (2D) Ruddlesden-Popper (RP) perovskites BA2FA(Pb1-xSnx)2I7 using a solution-based method. XRD study revealed the formation of orthorhombic phases for pristine (BA2FAPb2I7) and mixed Pb-Sn perovskite thin films. UV-vis analysis showed that different n = 2 and n = 3 phases are present in the pristine sample. In contrast, Pb-Sn-doped samples showed no signature of other phases with a prominent red-shift in the visible spectral region. Cyclic voltammetry showed peaks for electron transfers at the band edges. Additionally, electrochemical and optical band gap matching was observed, along with decreased peak intensity due to less reactant and altered electrolyte-perovskite interface stability. Density functional theory (DFT) calculations revealed that the reduced band gap is due to the alteration of electrostatic interactions and charge distribution within the lattice upon Sn substitution. Low-temperature PL analysis provided insights into charge carrier dynamics with Sn substitution and suggested the suppression of higher n phases and self-trapped excitons/carriers in mixed Pb-Sn quasi-2D RP perovskite thin films. This study sheds light on the electron transfer phenomena between TiO2 and SnO2 layers by estimating band offsets from valence band maximum (VBM) and conduction band minimum (CBM), which is crucial for future applications in fabricating stable and efficient 2D-Pb-Sn mixed perovskites for optoelectronic applications.
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