Metastable interphase induced pre-strain compensation enables efficient and stable perovskite solar cells†

Abstract

High-efficiency metal halide perovskite solar cells (PSCs) include rigid substrates with low thermal-expansion coefficients (TECs), resulting in significant TEC mismatch with the perovskites with high TECs at the buried interface. This mismatch leads to thermally induced residual tensile strain in perovskite films after annealing during film fabrication, which facilitates ion migration and defect formation, thereby compromising the performance and stability of PSCs. In this study, we present a pre-strain compensation strategy by introducing an in situ generated metastable Pb(CH₃NH₂)₂Cl₂ (PMC) phase at the buried substrate/perovskite interface, which will transform into PbCl₂ upon annealing of formamidinium lead iodide (FAPbI₃)-based perovskite films. This phase transformation provides a source of compressive stress for the perovskite films to counteract the adverse residual tensile strain during cooling from annealing. This strategy is demonstrated to be able to effectively reduce the defect formation and non-radiative recombination rates in the perovskite films, while enhancing the charge-carrier mobility, lowering the exciton binding energy, and weakening the electron–phonon coupling interactions. As a result, the corresponding modified n–i–p PSCs achieve a champion efficiency of 25.83% (certified at 25.36%) and exhibit improved stability.