Bias-Dependent Dynamics of Degradation and Recovery in Perovskite Solar Cells

Degradation of perovskite solar cells (PSCs) is often found to be partially or fully reversible when the cells are allowed to recover in the dark. Unlike the dynamics of degradation, knowledge about the dynamics of PSC cell recovery is very limited. Here, we demonstrate that the PSC recovery strongly depends on the electrical bias conditions during the light-induced degradation and that it can be manipulated by applying an external electrical bias during the recovery phase. Investigation of the recovery dynamics allows us to analyze the degradation mechanisms in detail. More specifically, we aged a mixed-cation mixed-halide PSC with a n-i-p structure under illumination in open-circuit (OC) or short-circuit (SC) conditions, and periodically measured their characteristics during the recovery. PSCs aged in SC degrade faster and fully recover after the light is switched off, while the performance of the cells aged in OC does not recover but instead further decreases after the light is switched off (drop-in-dark effect). With the use of transient photoluminescence, secondary ion mass spectrometry, and drift-diffusion-based simulations, we hypothesize that extrinsic ion migration causes the drop-in-dark effect, by forming an electron extraction barrier at the metal oxide electron transport layer. The applied bias alleviates this effect. Our results are relevant for gaining a deeper understanding of the multiple degradation mechanisms present in perovskite solar cells, and for finding a practical way to assist their recovery.

Automated summary

The recovery of perovskite solar cells strongly depends on the electrical bias conditions during light-induced degradation, and can be manipulated by applying external electrical bias. Cells aged under short-circuit conditions degrade faster but fully recover after light is switched off, while cells aged under open-circuit conditions do not recover and exhibit further performance decrease. Extrinsion ion migration is hypothesized to cause a drop-in-dark effect, which can be alleviated by applied bias.