Multidentate Chelation Achieves Bilateral Passivation toward Efficient and Stable Perovskite Solar Cells with Minimized Energy Losses.

Defects in the electron transport layer (ETL), perovskite, and buried interface will result in considerable nonradiative recombination. Here, a bottom-up bilateral modification strategy is proposed by incorporating arsenazo III (AA), a chromogenic agent for metal ions, to regulate SnO 2 nanoparticles. AA can complex with uncoordinated Sn 4+ /Pb 2+ in the form of multidentate chelation. Furthermore, by forming a hydrogen bond with formamidinium (FA), AA can suppress FA + defects and regulate crystallization. Multiple chemical bonds between AA and functional layers are established, synergistically preventing the agglomeration of SnO 2 nanoparticles, enhancing carrier transport dynamics, passivating bilateral defects, releasing tensile stress, and promoting the crystallization of perovskite. Ultimately, the AA-optimized power conversion efficiency (PCE) of the methylammonium-free (MA-free) devices (Rb 0.02 (FA 0.95 Cs 0.05 ) 0.98 PbI 2.91 Br 0.03 Cl 0.06 ) is boosted from 20.88% to 23.17% with a high open-circuit voltage ( V OC ) exceeding 1.18 V and ultralow energy losses down to 0.37 eV. In addition, the optimized devices also exhibit superior stability.