Tuning the Colloidal Softness of CsPbBr₃ Nanocrystals for Homogeneous Superlattices

Perovskite nanocrystal superlattices (NC SLs), made from millions of ordered crystals, support collective optoelectronic phenomena. Coupled NC emitters are highly sensitive to the structural and spectral inhomogeneities of the NC ensemble. Free electrons in scanning electron microscopy (SEM) are used to probe the cathodoluminescence (CL) properties of CsPbBr₃ SLs with a ∼20 nm spatial resolution. Correlated CL-SEM measurements allow for simultaneous characterization of structural and spectral heterogeneities of the SLs. Hyperspectral CL mapping shows multipole emissive domains within a single SL. Consistently, the edges of the SLs are blue-shifted relative to the central domain by up to 65 meV. We discover a relation between NC building block colloidal softness and the extent of the CL shift. Residual uniaxial compressive strains accompanying SL formation are contributors to these emission shifts. Therefore, precise control over the colloidal softness of the NC building blocks is critical for SL engineering.