Quadruple-Cation Wide-Bandgap Perovskite Solar Cells with Enhanced Thermal Stability Enabled by Vacuum Deposition

Vacuum processing of multicomponent perovskites is not straightforward, because the number of precursors is in principle limited by the number of available thermal sources. Herein, we present a process which allows increasing the complexity of the formulation of vacuum-deposited lead halide perovskite films by multisource deposition and premixing both inorganic and organic components. We apply it to the preparation of wide-bandgap CsMAFA triple-cation perovskite solar cells, which are found to be efficient but not thermally stable. With the aim of stabilizing the perovskite phase, we add guanidinium (GA⁺) to the material formulation and obtained CsMAFAGA quadruple-cation perovskite films with enhanced thermal stability, as observed by X-ray diffraction and rationalized by microstructural analysis. The corresponding solar cells showed similar performance with improved thermal stability. This work paves the way toward the vacuum processing of complex perovskite formulations, with important implications not only for photovoltaics but also for other fields of application.