A Universal Reverse-Cool Annealing Strategy Makes Two-Dimensional
Ruddlesden-Popper Perovskite Solar Cells Stable and Highly Efficient
with Voc Exceeding 1.2 V
Abstract
Two-dimensional Ruddlesden-Popper (2D RP) layered metal-halide
perovskites have garnered increasing attention due to their favorable
optoelectronic properties and enhanced stability in comparison to their
three-dimensional counterparts. Nevertheless, precise control over the
crystal orientation of 2D RP perovskite films remains challenging,
primarily due to the intricacies associated with the solvent evaporation
process. In this study, we introduce a novel approach known as
reverse-cool annealing (RCA) for the fabrication of 2D RP perovskite
films. This method involves a sequential annealing process at high and
low temperatures for wet perovskite films. The resulting RCA-based
perovskite films show the smallest root-mean-square value of 23.1 nm,
indicating a minimal surface roughness and a notably compact and smooth
surface morphology. The low defect density in these 2D RP perovskite
films with exceptional crystallinity suppresses non-radiative
recombination, leading to a minimal non-radiative open-circuit voltage
loss of 149 mV. Moreover, the average charge lifetime in these films is
extended to 56.30 ns, thanks to their preferential growth along the
out-of-plane direction. Consequently, the leading 2D RP perovskite solar
cell achieves an impressive power conversion efficiency of 17.8% and an
open-circuit voltage of 1.21 V. Additionally, the stability of the 2D RP
perovskite solar cell, even without encapsulation, exhibits substantial
improvement, retaining 97.4% of its initial efficiency after 1000 hours
under a nitrogen environment. The RCA strategy presents a promising
avenue for advancing the commercial prospects of 2D RP perovskite solar
cells.