Engineered CuInSe_<i>x</i>S_2–<i>x</i> Quantum Dots for Sensitized Solar Cells

Abstract

Colloidal CuInSe_<i>x</i>S_2–<i>x</i> quantum dots (QDs) are an attractive less-toxic alternative to PbX and CdX (X = S, Se, and Te) QDs for solution-processed semiconductor devices. This relatively new class of QD materials is particularly suited to serving as an absorber in photovoltaics, owing to its high absorption coefficient and near-optimal and finely tunable band gap. Here, we engineer CuInSe_<i>x</i>S_2–<i>x</i> QD sensitizers for enhanced performance of QD-sensitized TiO₂ solar cells (QDSSCs). Our QD synthesis employs 1-dodecanethiol (DDT) as a low-cost solvent, which also serves as a ligand, and a sulfur precursor; addition of triakylphosphine selenide leads to incorporation of controlled amounts of selenium, reducing the band gap compared to that of pure CuInS₂ QDs. This enables significantly higher photocurrent in the near-infrared (IR) region of the solar spectrum without sacrificing photovoltage. In order to passivate QD surface recombination centers, we perform a surface–cation exchange with Cd prior to sensitization, which enhances chemical stability and leads to a further increase in photocurrent. We use the synthesized QDs to demonstrate proof-of-concept QDSSCs with up to 3.5% power conversion efficiency