posted on 2023-12-06, 20:20authored byYong Wang, Shuming Ye, Ziwei Sun, Jiajun Zhu, Ye Liu, Rongfei Wang, Feng Lin, Wenhua Zhang, Yu Yang, Chong Wang
The fluorination of the aromatic multifunctional Lewis
base passivation
strategy has been demonstrated recently as an effective approach to
markedly enhance the performance of perovskite photovoltaic devices.
However, the regulation mechanisms of the passivation efficiency by
varying the functional group position of fluorine (F) in the regioisomers
have received little attention and inadequate research. Herein, a
pair of bifluorine-substituted aminobenzoic acid regioisomers [3-amino-2,6-difluorobenzoic
acid (13-FABA) and 4-amino-3,5-difluorobenzoic acid (14-FABA)] were
employed to investigate the passivation effects of Lewis bases dependent
on behaviors of the ortho/meta-substituted position of fluorine. The
density functional theory calculation on electron cloud density, interaction
energy, and the basicity of Lewis bases combined with experimental
evidence reveal that the ortho-effect induced by fluorine substitution
weakens the passivating effect of 13-FABA Lewis base and induces its
molecular propensity to form internal salts, accelerating the degradation
and deterioration of the device performance. Conversely, 14-FABA with
meta-connected fluorine atoms exhibit superior efficacy in suppressing
defects and enhancing hydrophobicity. Eventually, the 14-FABA-modified
photodetectors (PDs) achieved a high detectivity of 1.69 × 1013 Jones, the comparatively lower dark current density of 2.2
× 10–10 A/cm2 among all-inorganic
perovskite PD systems. Our work has not only clarified the fundamental
mechanisms of the F-substituted position effects of Lewis base on
suppressing defects but also provided a promising passivation strategy
for perovskite films via designing the regioisomeric atoms in a multifunctional
Lewis base molecule.