Defect Passivation of Organic–Inorganic Hybrid Perovskites by Diammonium Iodide toward High-Performance Photovoltaic Devices

The polycrystalline feature of solution-processed perovskite film and its ionic nature inevitably incur substantial crystallographic defects, especially at the film surface and the grain boundaries (GBs). Here, a simple defect passivation method was exploited by post-treating CH 3 NH 3 PbI 3 (MAPbI 3 ) film with a rationally selected diammonium iodide. The molecular structure of the used diammonium iodide was discovered to play a critical role in affecting the phase purity of treated MAPbI 3 . Both NH 3 I(CH 2 ) 4 NH 3 I and NH 3 I(CH 2 ) 2 O(CH 2 ) 2 NH 3 I (EDBE) induce three-dimensional (3D) to two-dimensional (2D) perovskite phase transformation during the treatment while only NH 3 I(CH 2 ) 8 NH 3 I (C8) successfully passivates perovskite surface and GBs without forming 2D perovskite because of the elevated activation energy arising from its unique anti–gauche isomerization. Defect passivation of MAPbI 3 was clearly confirmed by scanning Kelvin probe microscopy (SKPM) and time-resolved photoluminescence (TRPL) studies, which results in the reduced recombination loss in derived devices. Consequently, the perovskite solar cell with C8 passivation showed a much improved power conversion efficiency (PCE) of 17.60% compared to the control device PCE of 14.64%.