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Control over microstructures at the nanoscale (<100nm) still seems challenging due to, among other things, the stochastic nature of nucleation in the bulk phase. The densification of assemblies of ligand-capped nanocrystals (colloidal nanocrystal assemblies, CNAs) could bypass this challenge that limits our control over the nanostructure and, therefore, the properties of materials. However, the removal of the ligands and the cracking that follows it are the two critical hurdles that have been stymieing this approach. We show that low-pressure plasma processing can effectively remove ligands from CNAs (down to 0.6 at.% of carbon which can be accounted for adventitious carbon) without harming the properties of the inorganic cores of the nanoparticles and the structure of CNAs. The cracking of CNAs is correlated with the structure of the CNAs, which can be controlled and easily predicted by Hansen solubility parameters of solvent in which the nanoparticles are dispersed. While a fully solvated ligand shell leads to the formation of close-packed ordered CNAs – which cracked after selfassembly or ligand removal – a partially solvated one results in interdigitation of the ligand shell yielding disordered CNAs, which remained crack-free after ligand removal and sintering up to a critical cracking thickness of 440nm. The process is demonstrated with particles of different compositions, ligands, sizes, shapes, as well as with binary systems. These findings allowed for the fabrication of cm crack-free, phase-pure polycrystalline films with tunable, near-monodisperse grain sizes using CNAs as precursors. We observed electrical conductivities of PbS films produced by this

Bottom-up approach to fabricate nanostructured thin films from colloidal nanocrystal precursors