Structurally Flexible 2D Spacer for Suppressing the Electron-Phonon Coupling Induced Non-Radiative Decay in Perovskite Solar Cells

This study presents experimental evidence of the dependence of non-radiative recombination processes on the electron-phonon coupling of perovskite in perovskite solar cells(PSCs).Via A-site cation engineering,a weaker electron-phonon coupling in perovskite has been achieved by introducing the structurally soft cyclohexane methylamine(CMA^(+))cation,which could serve as a damper to alleviate the mechanical stress caused by lattice oscillations,compared to the rigid phenethyl methylamine(PEA^(+))analog.It demonstrates a significantly lower non-radiative recombination rate,even though the two types of bulky cations have similar chemical passivation effects on perovskite,which might be explained by the suppressed carrier capture process and improved lattice geometry relaxation.The resulting PSCs achieve an exceptional power conversion efficiency(PCE)of 25.5%with a record-high opencircuit voltage(V_(OC))of 1.20 V for narrow bandgap perovskite(FAPbI_(3)).The established correlations between electron-phonon coupling and non-radiative decay provide design and screening criteria for more effective passivators for highly efficient PSCs approaching the Shockley-Queisser limit.

Mechanical robust and self-healing flexible perovskite solar cells with efficiency exceeding 23%

Flexible perovskite solar cells(f-PSCs) have experienced rapid advancements due to the light-weight, flexibility, and solution processability of the perovskite materials, which prompted the power conversion efficiency(PCE) to 24.08%. However, f-PSCs still face challenges in terms of mechanical and environmental stability. This is primarily due to their inherent brittleness, the presence of residual tensile strain, and the high density of defects along the boundaries of perovskite grains. To this end, we carefully developed a cross-linkable elastomers 3-[(3-acrylamidopropyl)dimethylammonium] propanoate(ADP) with electrostatic dynamic bond, which could be in-situ cross-linked and coordinate with [Pb I6]4-to regulate the crystallization process of perovskite. The cross-linked elastomers attached to the perovskite grain boundaries could release the remaining tensile strains and mechanical stresses, leading to enhanced stability and flexibility of the f-PSCs. More importantly, the electrostatic interaction between positive and negative groups of cross-linked elastomers and hydrogen bond formation between N–H and C=O accelerate the cross-linking of ADP, endowing the flexible perovskite films with self-healing ability under mild treating conditions(60 °C for 30 min). As a result, the device achieves a remarkable PCE of 23.53%(certified 23.16%). Additionally, the device exhibits impressive mechanical sustainability and durability, retaining over 90% of initial PCE even after undergoing8,000 bending cycles.