The photophysical properties of methylammonium lead iodide (MAPbI3) quantum dots (QDs) have not been systematically studied for size and shape dependence. Here, we synthesize MAPbI3 QDs using ligand-assisted reprecipitation, controlling the injection speed and reaction times to produce QDs with different sizes and shapes. Dropwise injection yields ∼5 nm spherical QDs, emitting photoluminescence (PL) at 2.06 eV. In contrast, swift injections yield larger (>10 nm) rectangular QDs with varying aspect ratios, supported by an infinite quantum well model. The PL lifetime of QDs increases with their size, and the size variation significantly influences the ultra-low-frequency Raman modes at 81, 107, and 127 cm-1, in contrast to what is observed in polymorphic MAPbI3 thin films. Our findings, supported by first-principles density functional theory, show that key PL and Raman properties are governed by the sizes and shapes of MAPbI3 QDs. This study contributes to the understanding of the optical behavior of these QDs, which is crucial for their potential applications and environmental implications.
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