LAUSR

The ionic defects at the surfaces and grain boundaries of organic–inorganic halide perovskite films are detrimental to both the efficiency and stability of perovskite solar cells. Here, we show that quaternary ammonium halides can effectively passivate ionic defects in several different types of hybrid perovskite with their negative- and positive-charged components. The efficient defect passivation reduces the charge trap density and elongates the carrier recombination lifetime, which is supported by density-function-theory calculation. The defect passivation reduces the open-circuit-voltage deficit of the p–i–n-structured device to 0.39 V, and boosts the efficiency to a certified value of 20.59 ± 0.45%. Moreover, the defect healing also significantly enhances the stability of films in ambient conditions. Our findings provide an avenue for defect passivation to further improve both the efficiency and stability of solar cells. Losses in solar cells can be caused by material defects in the bulk or at interfaces. Here, Zheng et al. use quaternary ammonium halides to passivate various perovskite absorbers and prepare solar cells with certified efficiency above 20%, suggesting that both anionic and cation defects are affected.