Room-Temperature, Multigram-Scale Synthesis and Conversion Mechanism of Highly Luminescent Lead Sulfide Quantum Dots

J Phys Chem Lett. 2023 Sep 14;14(36):8129-8137. doi: 10.1021/acs.jpclett.3c02005. Epub 2023 Sep 5.

Abstract

PbS quantum dots (QDs) are attractive near-infrared (NIR) materials, but traditional synthetic methods require inert atmosphere and/or high temperature. Herein we develop a facile, room-temperature synthetic route for in situ halide passivated PbS QDs through controllable reactions between lead halide, N,N'-diphenyl thiourea, and oleyamine (OLA) in toluene. Contrast experiments and theoretical calculations reveal that the OLA plays a bifunctional role as a mild base to initiate the formation of PbS monomers and as a dynamic ligand to control the crystallization of PbS QDs and further ligand exchange. The oleic acid-capped PbS QDs exhibit high photoluminescence quantum yields up to 45%. The scaled-up synthesis on multigram scales shows great batch-to-batch consistency. We further demonstrate high-power NIR light-emitting diodes using the PbS QDs as color converters, delivering NIR optical power of 9.2 mW at 160 mA. This work provides a simple and versatile synthetic route for high-quality PbS QDs and boosts the applications of NIR materials.