Surface-capping engineering for electrically neutral surface of perovskite films and stable solar cells

Metal halide perovskite solar cells (PSCs) have developed rapidly in recent years, due to their high performance and low-cost solution-based fabrication process. These excellent properties are mainly attributed to the high defect tolerance of polycrystalline perovskite films. Meanwhile, these defects can also facilitate ion migration and carrier recombination, which cause the device performance and the long-term stability of PSCs to deteriorate heavily. Therefore, it is critical to passivate the defects, especially at the surfaces of perovskite grains where the defects are most concentrated due to the dangling bonds. Here we propose a surface-capping engineering (SCE) method to construct 'dangling-bond-free' surfaces for perovskite grains. Diamine iodide (methylenediammonium diiodide, MDAI₂) was used to construct an electroneutral PbX₆-MDA-PbX₆(X = Cl, Br or I) layer at the perovskite surfaces. Compared to the monovalent FA⁺which can only coordinate one [PbX₆]^4-slab, the bivalent MDA²⁺can coordinate two [PbX₆]^4-slabs on both sides, thus realizing a dangling-bond-free surface. Solar cells based on SCE-perovskite films exhibited a higher power conversion efficiency (PCE) of 21.6%, compared with 19.9% of the control group; and maintained over 96% of its initial PCE after 13 h during the maximum power point tracking test under continuous AM1.5G illumination, whereas the control group only lasted 1.5 h. Constructing a dangling-bond-free capping layer on the grain boundary opens new avenues for the fabrication of ultralow-defect polycrystalline semiconductors, paving the way to further improve the PCE and lifetime of PSCs.