Low-Cost, Air-Processed Quantum Dot Solar Cells via Diffusion-Controlled Synthesis

Despite significant advances in the development of high-efficiency and stable quantum dot (QD) solar cells (QDSCs), recent synthetic and fabrication routes still require improvements to render QDSCs commercially feasible. Here, we describe a low-cost, industrially viable fabrication method of QDSCs under an ambient atmosphere (humid air and room temperature) using stable, high-quality, and small-sized PbS QDs prepared with low-cost, greener precursors [i.e., thioacetamide (TAA)] compared to the widely used bis(trimethylsilyl)sulfide [(TMS)₂S], at low temperatures without requiring any stringent conditions. The low reaction temperature, medium reactivity of TAA, and diffusion-controlled particle growth adopted in this approach provide an opportunity to synthesize ultrasmall (emission peak ∼700 nm) to larger PbS QDs (emission peak ∼1050 nm). This also enables well-controlled large-scale (multigram) synthesis with a rough estimated production cost of PbS of 8.11 $ per gram (based on materials cost), which is the lowest among the available PbS QDs produced using wet chemistry routes. QDSCs fabricated using 3.25 nm PbS QDs (bandgap 1.29 eV) under ambient conditions yield a high circuit current density (J_sc) of 32.4 mA/cm² (one of the highest values of J_sc ever reported) with a power conversion efficiency of 7.8% under 1 sun simulated sunlight at AM 1.5 G (100 mW/cm²). These devices exhibit better photovoltaic performance compared to devices fabricated with more traditional PbS QDs synthesized with (TMS)₂S under an ambient atmosphere, confirming the quality of PbS QDs produced with our method. The diffusion-controlled TAA-based synthetic route developed herein is found to be very promising for synthesizing size-tunable PbS QDs for photovoltaic and other optoelectronic applications.