“…The forces that drive NC self-assembly range from hard- to soft-particle interactions. Taking advantage of previous knowledge gained on the self-assembly of conventional monodisperse colloidal NCs, a large variety of self-assembly techniques have been reported over the years such as evaporation-driven or destabilization-driven approaches, as well as spontaneous and template-assisted self-assembly. ,, Recently, these techniques have been extended to self-assembly of halide perovskite NCs into highly ordered SLs for exploration of their collective properties that can be very different from their individual constituents. ,,,,,,,− Near monodispersity of NCs and high shape uniformity are important factors to obtain long-range ordered NC SLs. ,, Fortunately, these conditions are easily met for all-inorganic CsPbX 3 perovskite NCs as they are often prepared with near monodispersity regardless of the synthesis method, as discussed in the synthesis section. ,,,, As a result, these perovskite nanocubes tend to self-assemble into 1D or 2D SLs on a TEM grid upon solvent evaporation from a droplet of high concentrated colloidal solution. Initial examples of CsPbBr 3 nanocube SLs date back to 2017, when 2D and 3D assemblies were obtained by the solvent evaporation method. ,, In reference small superlattice domains on TEM grids exhibit a simple cubic packing of the nanocubes with a lattice constant of ≈12.5 nm and an interparticle separation of ≈2.3 nm.…”