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

Author:

Lapkin DmitryORCID,Kirsch Christopher,Hiller JonasORCID,Andrienko DenisORCID,Assalauova Dameli,Braun Kai,Carnis JeromeORCID,Kim Young YongORCID,Mandal Mukunda,Maier Andre,Meixner Alfred J.ORCID,Mukharamova Nastasia,Scheele MarcusORCID,Schreiber FrankORCID,Sprung Michael,Wahl Jan,Westendorf Sophia,Zaluzhnyy Ivan A.,Vartanyants Ivan A.ORCID

Abstract

AbstractWe correlate spatially resolved fluorescence (-lifetime) measurements with X-ray nanodiffraction to reveal surface defects in supercrystals of self-assembled cesium lead halide perovskite nanocrystals and study their effect on the fluorescence properties. Upon comparison with density functional modeling, we show that a loss in structural coherence, an increasing atomic misalignment between adjacent nanocrystals, and growing compressive strain near the surface of the supercrystal are responsible for the observed fluorescence blueshift and decreased fluorescence lifetimes. Such surface defect-related optical properties extend the frequently assumed analogy between atoms and nanocrystals as so-called quasi-atoms. Our results emphasize the importance of minimizing strain during the self-assembly of perovskite nanocrystals into supercrystals for lighting application such as superfluorescent emitters.

Funder

Deutsche Forschungsgemeinschaft

Russian Science Foundation

Helmholtz Association

Publisher

Springer Science and Business Media LLC

Subject

General Physics and Astronomy,General Biochemistry, Genetics and Molecular Biology,General Chemistry,Multidisciplinary

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