Abstract
Using reduced-dimensional halide perovskites is emerging as a promising strategy for enhancing the stability of optoelectronic devices such as solar cells, even if their performances remain a step below those of the 3D halide perovskites. Two-dimensional Ruddlesden-Popper (2D-RP) structures are characterized by the n parameter that represents the number of PbI(6) layers in the spacer-separated perovskite slabs. The present study focuses on formamidinium (FA)-based 2D-RP type perovskites denoted as PMA(2)FA(n-1)Pb(n)I(3n+1) (PMA = Phenylmethylammonium or benzylammonium). We investigate the effect of n on the one step growth mechanism and the film morphology, microstructure, phase purity, and optoelectronic properties. Our findings demonstrate that the average n is not only determined by the initial spacer content in the precursor solution but also by the thermal annealing process that leads to a partial spacer loss. Depending on n, perovskite solar cells achieving a power conversion efficiency up to 21%, coupled with enhanced film stability compared to 3D perovskites have been prepared. By using MACl additive and an excess of PbI(2) in the perovskite precursor solution, we have been able to achieve high efficiency and to stabilize the n = 5 perovskite solar cells. This research represents a significant stride in comprehending the formation of FA-based layered perovskites through one-step sequential deposition, enabling control over their phase distribution, composition, and orientation.