Tetrafluoroborate-Induced Reduction In Defect Density In Hybrid Perovskites Through Halide Management
ADVANCED MATERIALS(2021)
Abstract
Hybrid-perovskite-based optoelectronic devices are demonstrating unprecedented growth in performance, and defect passivation approaches are highly promising routes to further improve properties. Here, the effect of the molecular ion BF4-, introduced via methylammonium tetrafluoroborate (MABF(4)) in a surface treatment for MAPbI(3) perovskite, is reported. Optical spectroscopy characterization shows that the introduction of tetrafluoroborate leads to reduced non-radiative charge-carrier recombination with a reduction in first-order recombination rate from 6.5 x 10(6) to 2.5 x 10(5) s(-1) in BF4--treated samples, and a consequent increase in photoluminescence quantum yield by an order of magnitude (from 0.5 to 10.4%). F-19, B-11, and N-14 solid-state NMR is used to elucidate the atomic-level mechanism of the BF4- additive-induced improvements, revealing that the BF4- acts as a scavenger of excess MAI by forming MAI-MABF(4) cocrystals. This shifts the equilibrium of iodide concentration in the perovskite phase, thereby reducing the concentration of interstitial iodide defects that act as deep traps and non-radiative recombination centers. These collective results allow us to elucidate the microscopic mechanism of action of BF4-.
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Key words
charge-carrier recombination, defects, perovskite solar cells, photoluminescence, surface treatment, tetrafluoroborate
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