A Novel Multiple-Ring Aromatic Spacer Based 2D Ruddlesden-Popper CsPbI3 Solar Cell with Record Efficiency Beyond 16%

Two-dimensional (2D) Ruddlesden-Popper (RP) CsPbI3 perovskite possesses superior phase stability by introducing steric hindrance. However, due to the quantum and dielectric confinement effect, 2D structures usually exhibit large exciton binding energy, and the charge tunneling barrier across the organic interlayer is difficult to eliminate, resulting in poor charge transport and performance. Here, a multiple-ring aromatic ammonium, 1-naphthylamine (1-NA) spacer is developed for 2D RP CsPbI3 perovskite solar cell (PSC). Theoretical simulations and experimental characterizations demonstrate that the 2D RP CsPbI3 perovskite using 1-NA spacer with extended pi-conjugation lengths reduces the exciton binding energy and facilitates the efficient separation of excitons. In addition, its cations have a significant contribution to the conduction band, which can reduce the bandgap, promote electronic coupling between organic and inorganic layers, and improve interlayer charge transport. Importantly, the strong pi-pi conjugation of 1-NA spacer can enhance intermolecular interactions and hydrogen bonding, and prepare high-quality films with preferred vertical orientation, resulting in lower defect density, and directional charge transport. As a result, the (1-NA)(2)(Cs)(3)Pb4I3 PSC exhibits a record 16.62% performance with enhanced stability. This work provides an efficient approach to improve charge transport and device performance by developing multiple-ring aromatic spacers.

Automated summary

In this study, a novel approach to improve charge transport and device performance in two-dimensional RP CsPbI3 perovskite solar cells (PSC) was proposed by developing a multiple-ring aromatic spacer. The use of 1-naphthylamine (1-NA) spacer with extended pi-conjugation lengths was found to reduce the exciton binding energy and facilitate efficient separation of excitons. The cations of the spacer also made a significant contribution to the conduction band, leading to a reduced bandgap and improved interlayer charge transport. The strong pi-pi conjugation of the spacer enhanced intermolecular interactions and hydrogen bonding, resulting in high-quality films with preferred vertical orientation and lower defect density. The (1-NA)(2)(Cs)(3)Pb4I3 PSC achieved a record 16.62% performance with enhanced stability.