Diffusion-Controlled Synthesis of PbS and PbSe Quantum Dots with <i>in Situ</i> Halide Passivation for Quantum Dot Solar Cells

Abstract

We developed a simple non-hot-injection synthetic route that achieves in situ halide-passivated PbS and PbSe quantum dots (QDs) and simplifies the fabrication of Pb-chalcogenide QD solar cells. The synthesis mechanism follows a temperature-dependent diffusion growth model leading to strategies that can achieve narrow size distributions for a range of sizes. We show that PbS QDs can be produced with a diameter as small as 2.2 nm, corresponding to a 1.7 eV band gap, while the resulting size distribution (6-7%) is comparable to that of hot-injection syntheses. The in situ chloride surface passivation is demonstrated by X-ray photoelectron spectroscopy and an improved photostability of both PbS and PbSe QDs when stored under air. Additionally, the photoluminescence quantum yield of the PbS QDs is ∼30% higher compared to the traditional synthesis. We show that PbS QD solar cells with 6.5% power conversion efficiency (PCE) can be constructed. Finally, we fabricated PbSe QD solar cells in air (rather than in inert atmosphere), achieving a PCE of 2.65% using relatively large QDs with a corresponding band gap of 0.89 eV.