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Point defect tolerance in materials, which extends operational lifetime, isessential for societal sustainability, and the creation of a framework todesign such properties is a grand challenge in the material sciences. Usingthree prototypical lead bromide perovskites in single crystal form andhigh-resolution synchrotron-based X-ray spectroscopy, we reveal theunexpectedly pivotal role of the A-cation in mediating the influence ofphotoinduced defects. Organic A-cation hydrogen bonding facilitates chemicalflexing of the lead-bromide bond that mitigates the self-doping effect ofbromide vacancies. The contribution of partially ionic lead-bromide bonding tothe electronic band edges, where the bonding becomes more ionic upon theformation of defects, mitigates re-hybridization of the electronic structureupon degradation. These findings reveal two new general design principles fordefect tolerance in materials. Our findings uncover the foundations of defecttolerance in halide perovskites and have implications for defect calculations,all beam-based measurements of photophysical properties and perovskite solarcell technology.

Experimentally observed defect tolerance in the electronic structure of lead bromide perovskites