Simultaneous Enhancement of Efficiency And Operational-Stability of Mesoscopic Perovskite Solar Cells via Interfacial Toughening: Article No. 2308819

We have investigated the combined effects of compact TiO2 (c-TiO2) electron-transport layer (ETL) without and with mesoscopic TiO2 (m-TiO2) on top, and without and with an iodine-terminated silane self-assembled monolayer (SAM), on the mechanical behavior, opto-electronic properties, photovoltaic (PV) performance, and operational-stability of solar cells based on metal-halide perovskites (MHPs). The interfacial toughness increases almost three-fold in going from c-TiO2 without SAM to m-TiO2 with SAM. This is attributed to the synergistic effect of the m-TiO2/MHP nanocomposite at the interface and the enhanced adhesion afforded by the iodine-terminated silane SAM. The combination of m-TiO2 and SAM also offers a significant beneficial effect on the photocarriers extraction at the ETL/MHP interface, resulting in perovskite solar cells (PSCs) with power-conversion efficiency (PCE) of over 24% and 20% for 0.1 cm2 and 1 cm2 active areas, respectively. These PSCs also have exceptionally long operational-stability lives: extrapolated T80 (duration at 80% initial PCE retained) is about 18,000 h and 10,000 h for 0.1 cm2 for 1 cm2 active areas, respectively. Postmortem characterization and analyses of the operational-stability-tested PSCs were performed to elucidate the possible mechanisms responsible for the long operational-stability.