Caesium-Iodide-Assisted Synthesis of High-Quality, Stable, and Robust Lead-Free Perovskite Quantum Dots

Abstract

The poor morphology, and susceptibility to oxidation of tin-based perovskite quantum dots (TQDs) have posed significant challenges, limiting their application potential. This study presents a straightforward method for synthesizing high-quality CsSnI3-based perovskite quantum dots (TQDs) by incorporating a mixed Cs source of Cs2CO3 and CsI. The addition of CsI increased the I:Sn ratio while maintaining Sn:Cs, resulting in TQDs with smaller size and improved uniformity. X-ray photoelectron spectroscopy (XPS), and Nuclear magnetic resonance (NMR) analyses confirmed enhanced crystallinity, photoluminescence intensity, and antioxidation ability of CsI-TQDs. Remarkably, these TQDs exhibit exceptional stability, enduring over 1 h in air and more than 24 h before complete oxidation, surpassing the previously reported longest lifetime in air for TQDs with conventional oleic acid (OA) and oleylamine (OAm) ligands. Furthermore, these TQD films retain robustness after ligand exchange with methyl acetate (MeOAc) and formamidinium iodide (FAI), representing the first successful short-ligand exchange of TQDs and enabling further electronic device applications. These findings suggest that CsI in the Cs source plays a crucial role in facilitating the formation of surface complexes, regulating TQD growth and suppressing iodine vacancies.