Open‐Shell Diradical‐Sensitized Electron Transport Layer for High‐Performance Colloidal Quantum Dot Solar Cells

Abstract The zinc oxide (ZnO) nanoparticles (NPs) are well‐documented as an excellent electron transport layer (ETL) in optoelectronic devices. However, the intrinsic surface flaw of the ZnO NPs can easily result in serious surface recombination of carriers. Exploring effective passivation methods of ZnO NPs is essential to maximize the device's performance. Herein, a hybrid strategy is explored for the first time to improve the quality of ZnO ETL by incorporating stable organic open‐shell donor‐acceptor type diradicaloids. The high electron‐donating feature of the diradical molecules can efficiently passivate the deep‐level trap states and improve the conductivity of ZnO NP film. The unique advantage of the radical strategy is that its passivation effectiveness is highly correlated with the electron‐donating ability of radical molecules, which can be precisely controlled by the rational design of molecular chemical structures. The well‐passivated ZnO ETL is applied in lead sulfide (PbS) colloidal quantum dot solar cells, delivering a power conversion efficiency of 13.54%. More importantly, as a proof‐of‐concept study, this work will inspire the exploration of general strategies using radical molecules to construct high‐efficiency solution‐processed optoelectronic devices.