Ligand‐Mediated Homojunction Structure for High‐Efficiency FAPbI3 Quantum Dot Solar Cells

Abstract Formamidinium lead iodide quantum dots (QDs) show great potential for solar cell applications but suffer from restricted charge transfer due to the insulating nature of their ligand shell. Management of the surface properties and resultant energy band alignment is the key to efficient and stable QD solar cells. Herein, an advance in QD surface passivation by introducing tailored multifunctional ligands (glycocyamine (GLA)) to the FAPbI 3 QD surface is demonstrated. The incorporation of GLA ligands can partly substitute the native long‐chain insulating ligands and effectively reduce the non‐radiative recombination loss induced by surface trap states. Notably, the introduction of GLA ligands beneficially shifts the band offsets of the QD films and generates a homojunction structure with a cascading energy band alignment in the QD layers, promoting favorable charge transport and boosting the device's performance. As a result, a record‐high power conversion efficiency (PCE) of 15.34% with improved open‐circuit voltage and fill factor is achieved. Moreover, the GLA‐assisted surface passivation boosts the device stability, in which over 80% and 75% of the original PCEs are maintained after storing the devices for 5500 h in ambient air and 768 h under continuous 1‐sun illumination, respectively.