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The synthesis of metal sulfide nanocrystals is a crucial step in the fabrication of quantum dot (QD) photovoltaics. Control over the QD size during synthesis allows for precise tuning of their optical and electronic properties, making them an appealing choice for electronic applications. This flexibility has led to the implementation of QDs in both highly‐efficient single junction solar cells and other optoelectronic devices including photodetectors and transistors. Most commonly, metal sulfide QDs are synthesized using the hot‐injection method utilizing a toxic, and air‐ and moisture‐sensitive sulfur source: bis(trimethylsilyl) sulfide ((TMS)2S). Here, bis(stearoyl) sulfide (St2S) is presented as a new type of air‐stable sulfur precursor for the synthesis of sulfide‐based QDs, which yields uniform, pure, and stable nanocrystals. Photovoltaic devices based on these QDs are equally efficient as those fabricated by (TMS)2S but exhibit enhanced operational stability. These results highlight that St2S can be widely adopted for the synthesis of metal sulfide QDs for a range of optoelectronic applications. [ABSTRACT FROM AUTHOR]

Light‐harvesting devices made from lead sulfide quantum dot (QD) absorbers are one of the many promising technologies of third‐generation photovoltaics. Their simple, solution‐based fabrication, together with a highly tunable and broad light absorption makes their application in newly developed solar cells, particularly promising. In order to yield devices with reduced voltage and current losses, PbS QDs need to have strategically passivated surfaces, most commonly achieved through lead iodide and bromide passivation. The interdot spacing is then predominantly filled with residual amorphous lead halide species that remain from the ligand exchange, thus hindering efficient charge transport and reducing device stability. Herein, it is demonstrated that a post‐treatment by iodide‐based 2‐phenylethlyammonium salts and intermediate 2D perovskite formation can be used to manage the lead halide excess in the PbS QD active layer. This treatment results in improved device performance and increased shelf‐life stability, demonstrating the importance of interdot spacing management in PbS QD photovoltaics. [ABSTRACT FROM AUTHOR]