Sequential Co-Passivation in InAs Colloidal Quantum Dot Solids Enables Efficient Near-Infrared Photodetectors.

III-V colloidal quantum dots (CQDs) are promising materials for optoelectronic applications, for they avoid heavy metals while achieving absorption spanning the visible to the infrared. However, the covalent nature of III-V CQDs requires the development of new passivation strategies to fabricate conductive CQD solids for optoelectronics: we show herein that ligand exchanges, previously developed in II-VI and IV-VI quantum dots and employing a single ligand, do not fully passivate CQDs, and that this curtails device efficiency. Guided by density functional theory (DFT) simulations, we develop a co-passivation strategy to fabricate indium arsenide CQD photodetectors, an approach that employs the combination of X-type methyl ammonium acetate (MaAc) and Z-type ligands InBr 3 . This approach maintains charge carrier mobility and improves passivation, seen in a 25% decrease in Stokes shift, a four-fold reduction in the rate of first-exciton absorption linewidth broadening over time-under-stress, and leads to a doubling in photoluminescence lifetime. The resulting devices show 37% external quantum efficiency at 950 nm, the highest value reported for InAs CQD photodetectors. This article is protected by copyright. All rights reserved.