Interfacial Degradation of Planar Lead Halide Perovskite Solar Cells

TLDR

The stability of perovskite solar cells is a major barrier to commercialization, with water identified as a key degradation source. This work investigates how different cathode metal contacts in ITO/PEDOT:PSS/MAPbI₃/PCBM/Metal devices affect performance loss under 4 h of steady illumination, reducing efficiency from 12 % to 1.8 %. Using capacitance–voltage, X‑ray diffraction, and optical absorption, the authors show that the bulk perovskite remains largely intact while the cathode contact undergoes chemical and electrical changes. They find that degradation is driven by chemical reactions at the metal contact that generate a dipole, shift the flat‑band potential, and hinder electron extraction; Cr₂O₃/Cr contacts improve stability but alter the energy profile, underscoring the need for protective layers to mitigate perovskite–contact reactivity.

Abstract

The stability of perovskite solar cells is one of the major challenges for this technology to reach commercialization, with water believed to be the major degradation source. In this work, a range of devices containing different cathode metal contacts in the configuration ITO/PEDOT:PSS/MAPbI3/PCBM/Metal are fully electrically characterized before and after degradation caused by steady illumination during 4 h that induces a dramatic reduction in power conversion efficiency from values of 12 to 1.8%. We show that a decrease in performance and generation of the S-shape is associated with chemical degradation of the metal contact. Alternatively, use of Cr2O3/Cr as the contact enhances the stability, but modification of the energetic profile during steady illumination takes place, significantly reducing the performance. Several techniques including capacitance–voltage, X-ray diffraction, and optical absorption results suggest that the properties of the bulk perovskite layer are little affected in the device degradation process. Capacitance–voltage and impedance spectroscopy results show that the electrical properties of the cathode contact are being modified by generation of a dipole at the cathode that causes a large shift of the flat-band potential that modifies the interfacial energy barrier and impedes efficient extraction of electrons. Ionic movement in the perovskite layer changes the energy profile close to the contacts, modifying the energy level stabilization at the cathode. These results provide insights into the degradation mechanisms of perovskite solar cells and highlight the importance to further study the use of protecting layers to avoid the chemical reactivity of the perovskite with the external contacts.