High-density
and multitype surface defects of CsPbI2Br perovskite induce
charge recombination and accumulation, hindering
its device efficiency and stability. However, the surface defect types
of CsPbI2Br perovskite are still unclear, and conventional
organic molecules only passivate one specific defect and cannot achieve
good overall passivation. Here, density functional theory is used
to explore surface defect types and properties of CsPbI2Br with calculating the defect formation energy and electronic structure.
Results show that the dominant deep-level defects are cationic defects
(PbBr) under Br-poor conditions and anionic defects (Ii and Bri) under moderate and Br-rich conditions,
originating from Pb–Pb bonding and I–I bonding. Multifunctional
organic molecules containing donor and acceptor groups are used to
passivate both cationic and anionic defects simultaneously. It turns
out that the deep-level defects are effectively decreased by forming
strong interaction of N–Pb, O–Pb, and halide–Pb
bonds. Moreover, the electron and hole transfers from perovskite to
molecules increase dramatically to −9.06 × 1012 and 2.60 × 1012
e/cm2 and maybe improve the efficiency of power conversion. Our findings
not only reveal the surface defect properties of CsPbI2Br, but also offer an approach for designing new multifunctional
passivators for perovskite solar cells with high conversion efficiency.