Multifaceted Characterization Methodology for Understanding Nonidealities in Perovskite Solar Cells: A Passivation Case Study

A multifaceted characterization approach is proposed, aiming to establish a link between nanoscale electrical properties and macroscale device characteristics. Current–voltage (I–V) measurements are combined with admittance spectroscopy (AS) and deep‐level transient spectroscopy (DLTS) for the analysis of charge‐related performance losses with time‐of‐flight secondary‐ion mass spectrometry to complete the understanding of ionic motion in the device. This is applied to the study of surface treatment in perovskite solar cells, which implements several strategies to improve band alignment, perovskite grain growth, and chemical passivation. An increase of both open‐circuit voltage (V_oc) and fill factor of respectively 90 mV and 11% is shown after surface treatment, with an absolute efficiency increase of 4%. AS measurements, coupled with a lumped elements model, rule out the impact of transport layers as the origin of the performance improvement, rather pointing toward a reduction in ionic resistance in the perovskite bulk. Analysis of the DLTS response yields an activation energy of 0.41 eV, which is likely related to the same ionic mechanism discovered with AS. Finally, both of these techniques enable to show that the surface treatment main contribution is to reduce ion‐related recombination of charge carriers.