Regulation of the quantum barrier and carrier transport toward high-efficiency quasi-2D Dion-Jacobson tin perovskite solar cells

Abstract

Quasi-2D Dion-Jacobson (DJ) tin halide perovskite has attracted much attention due to its elimination of Van der Waals gap and enhanced environmental stability. However, the bulky organic spacers usually form a natural quantum well structure, which brings a large quantum barrier and poor film quality, further limiting the carrier transport and device performance. Here, we designed three organic spacers with different chain lengths (ethylenediamine (EDA), 1,3-propanediamine (PDA), and 1,4-butanediamine (BDA)) to investigate the quantum barrier dependence. Theoretical and experimental characterizations indicate that EDA with short chain can reduce the lattice distortion and dielectric confinement effect, which is beneficial to the effective dissociation of excitons and the inhibition of trap-free non-radiative relaxation. In addition, EDA cation shows strong interaction with the inorganic octahedron, realizing large aggregates in precursor solution and high-quality films with improved structural stability. Furthermore, femtosecond transient absorption proves that EDA cations can also weaken the formation of small n-phases with large quantum barrier to achieve effective carrier transport between different n-phases. Finally, the quasi-2D DJ (EDA)FA9Sn10I31 solar cells achieves a 7.07% power conversion efficiency with good environment stability. Therefore, this work sheds light on the regulation of the quantum barrier and carrier transport through the chain length of organic spacer for quasi-2D DJ lead-free perovskites.