Highly Luminescent Phase-Stable CsPbI_3 Perovskite Quantum Dots Achieving Near 100 Absolute Photoluminescence Quantum Yieldand Applications to Solar Cells

摘要

Perovskite quantum dots (QDs) as a new type of colloidal nanocrystals have gained significant attention for both fundamental research and commercial applications owing to their appealing optoelectronic properties and excellent chemical processability. For their wide range of potential applications, synthesizing colloidal QDs with high crystal quality is of crucial importance. However, like most common QD systems, those reported perovskite QDs still suffer from a certain density of trapping defects, giving rise to detrimental non-radiative recombination centers and thus quenching luminescence. In this study, we show that a high room-temperature photoluminescence quantum yield (PL QY) of up to 100% can be obtained in CsPbI_3 perovskite QDs, signifying the achievement of almost complete elimination of the trapping defects. This is realized with our improved synthetic protocol that involves introducing organolead compound trioctylphosphine-PbI_3 (TOP-PbI_3) as the reactive precursor, which also leads to a significantly improved stability for the resulting CsPbI_3 QD solutions. Ultrafast kinetic analysis with time-resolved transient absorption spectroscopy evidences the negligible electron or hole trapping pathways in our QDs, which explains such a high quantum efficiency. We expect the successful synthesis of the "ideal" perovskite QDs will exert profound influence on their applications to both QD-based light-harvesting and -emitting devices.