Although β-CsPbI3 has a bandgap favorable for application in tandem solar cells, depositing and stabilizing β-CsPbI3 experimentally has remained a challenge. We obtained highly crystalline β-CsPbI3 films with an extended spectral response and enhanced phase stability. Synchrotron-based x-ray scattering revealed the presence of highly oriented β-CsPbI3 grains, and sensitive elemental analyses-including inductively coupled plasma mass spectrometry and time-of-flight secondary ion mass spectrometry-confirmed their all-inorganic composition. We further mitigated the effects of cracks and pinholes in the perovskite layer by surface treating with choline iodide, which increased the charge-carrier lifetime and improved the energy-level alignment between the β-CsPbI3 absorber layer and carrier-selective contacts. The perovskite solar cells made from the treated material have highly reproducible and stable efficiencies reaching 18.4% under 45 ± 5°C ambient conditions.
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