Ionic Liquid Treatment for Highest-Efficiency Ambient Printed Stable All-Inorganic CsPbI 3 Perovskite Solar Cells.

All-inorganic cesium lead triiodide (CsPbI 3 ) perovskite is well known for its unparalleled stability at high temperatures up to 500 °C and under oxidative chemical stresses. However, upscaling solar cells via ambient printing suffers from imperfect crystal quality and defects caused by uncontrollable crystallization. Here, the incorporation of a low concentration of novel ionic liquid is reported as being promising for managing defects in CsPbI 3 films, interfacial energy alignment, and device stability of solar cells fabricated via ambient blade-coating. Both theoretical simulations and experimental measurements reveal that the ionic liquid successfully regulates the perovskite thin-film growth to decrease perovskite grain boundaries, strongly coordinates with the undercoordinated Pb 2+ to passivate iodide vacancy defects, aligns the interface to decrease the energy barrier at the electron-transporting layer, and relaxes the lattice strain to promote phase stability. Consequently, ambient printed CsPbI 3 solar cells with power conversion efficiency as high as 20.01% under 1 sun illumination (100 mW cm -2 ) and 37.24% under indoor light illumination (1000 lux, 365 µW cm -2 ) are achieved; both are the highest for printed all-inorganic cells for corresponding applications. Furthermore, the bare cells show an impressive long-term ambient stability with only ≈5% PCE degradation after 1000 h aging under ambient conditions.