Interface Reactive Sputtering of Transparent Electrode for High‐Performance Monolithic and Stacked Perovskite Tandem Solar Cells

Abstract Sputtered indium tin oxide (ITO) fulfills the requirements of top transparent electrodes (TTEs) in semitransparent perovskite solar cells (PSCs) and stacked tandem solar cells (TSCs), as well as of the recombination layers in monolithic TSCs. However, the high‐energy ITO particles will cause damage to the devices. Herein, the interface reactive sputtering strategy is proposed to construct cost‐effective TTEs with high transmittance and excellent carrier transporting ability. Polyethylenimine (PEI) is chosen as the interface reactant that can react with sputtered ITO nanoparticles, so that, coordination compounds can be formed during the deposition process, facilitating the carrier transport at the interface of C₆₀/PEI/ITO. Besides, the impact force of energetic ITO particles is greatly alleviated, and the intactness of the underlying C₆₀ layer and perovskite layer is guaranteed. Thus, the prepared semitransparent subcells achieve a significantly enhanced power conversion efficiency (PCE) of 19.17%, surpassing those based on C₆₀/ITO (11.64%). Moreover, the PEI‐based devices demonstrate excellent storage stability, which maintains 98% of their original PCEs after 2000 h. On the strength of the interface reactive sputtering ITO electrode, a stacked all‐perovskite TSC with a PCE of 26.89% and a monolithic perovskite–organic TSC with a PCE of 24.33% are successfully fabricated.