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We correlate spatially resolved fluorescence (-lifetime) measurements withX-ray nanodiffraction to reveal surface defects in supercrystals ofself-assembled caesium lead halide perovskite nanocrystals and study theireffect on the fluorescence properties. Upon comparison with density functionalmodelling, we show that a loss in structural coherence, an increasing atomicmisalignment between adjacent nanocrystals, and growing compressive strain nearthe surface of the supercrystal are responsible for the observed fluorescenceblueshift and decreased fluorescence lifetimes. Such surface defect-relatedoptical properties extend the frequently assumed analogy between atoms andnanocrystals as so-called quasi-atoms. Our results emphasize the importance ofminimizing strain during the self-assembly of perovskite nanocrystals intosupercrystals for lighting application such as superfluorescent emitters.

Spatially resolved fluorescence of caesium lead halide perovskite supercrystals reveals quasi-atomic behavior of nanocrystals