We compare the fluorescence properties of CsPbBr2Cl nanocrystals, obtained via two distinct synthetic procedures and self-assembled into supercrystals using the same antisolvent crystallization technique. By spatially resolved fluorescence (lifetime) measurements we demonstrate that the optical properties of the supercrystals depend on the specific synthesis conditions of the constituting nanocrystals. Using scanning electron microscopy, small-angle X-ray scattering, and nuclear magnetic resonance spectroscopy, we find evidence that spatial fluctuations in the supercrystal fluorescence correlate with the ligand sphere of the nanocrystals. Specifically, homogeneous surface passivation of the nanocrystals leads to consistent interparticle distances and increased structural order within the supercrystals, resulting in a uniform fluorescence center wavelength and lifetime. The results of this study emphasize the importance of the relationship between crystalline structure and ligand configuration in controlling the optical properties of lead halide perovskite supercrystals.
Thalwitzer et al. (Wed,) studied this question.