Predicting Long-Term Stability from Short-Term Measurement: Insights from Modeling Degradation in Perovskite Solar Cells during Voltage Scans and Impedance Spectroscopy

A drift-diffusion model is used to investigate the effect of device degradation on current-voltage and impedance measurements of perovskite solar cells (PSCs). Modifications are made to the open-source drift-diffusion software IonMonger to model degradation via an increasing recombination rate during the course of characterization experiments. Impedance spectroscopy is shown to be a significantly more sensitive measure of degradation than current-voltage curves, reliably detecting a power conversion efficiency drop of as little as 0.06% over a 4 h measurement. Furthermore, we find that fast degradation occurring during impedance spectroscopy can induce loops lying above the axis in the Nyquist plot, the first time this experimentally observed phenomenon has been replicated in a physics-based model.