Cesium
formadinium methylammonium triple-cation (CsFAMA) lead mixed-halide
perovskites have been reported to promote unique photovoltaic properties
with high efficiency and minimal hysteresis effects. Perovskite film
quality is a vital parameter for improving the performance of perovskite
solar cells (PSCs). Here, we report the growth of CsFAMA perovskites
with microscale grains passivation grain boundaries by mixing HC(NH2)2I (FAI) and CH3NH3Br (MABr)
in isopropanol (IPA) as a post-treatment step to cause controlled
Ostwald ripening, leading to secondary grain growth. Compared to the
conventional preparation of perovskite films with a free organic halide
antisolvent, this mixed-cation mixed-halide post-treatment created
higher quality perovskite films in terms of morphology, electronic
properties, energy level alignment, and carrier recombination, with
the band gap adjusted at the optimal concentration. Treatment with
the single cation and single halide presented by FAI and/or MABr in
IPA treatment was also investigated, and the results showed that multiple
band gap perovskite structures were obtained, which could be beneficial
for band gap engineering. This method of perovskite preparation was
tested in an inverted planar configuration with a hole transport layer
(HTL) based on sulfonated poly(thiophene-3-[2-(2-methoxy-ethoxy)ethoxy]-2,5-diyl)
(SP3MEET). The efficiency of the PSCs was dramatically boosted from
13.80% with the organic halide-free antisolvent to 17.62% when the
mixed-cation mixed-halide approach was used. In addition, the PSCs
treated with the mixed-cation mixed-halide solution exhibited excellent
reproducibility, with a high fill factor and eliminated hysteresis.
The CsFAMA photovoltaic device based on the single organic cation
and single halide treatment approach showed power conversion efficiency
of 15.82 and 15.90% for the FAI and MABr-treated films, respectively.
Characterization of the S-P3MEET as HTLs found that good optoelectronic
and morphological properties lead to improve the performance of the
inverted PSC. However, with further research to align the energy levels
at the S-P3MEET/perovskite interface, greater improvements in the
PSCs are expected.