Self-assembly of nanocrystals into strongly electronically coupled all- inorganic supercrystals

I Coropceanu and EM Janke and J Portner and D Haubold and TD Nguyen and A Das and CPN Tanner and JK Utterback and SW Teitelbaum and MH Hudson and NA Sarma and AM Hinkle and CJ Tassone and A Eychmuller and DT Limmer and MO de la Cruz and NS Ginsberg and DV Talapin, SCIENCE, 375, 1422-+ (2022).

DOI: 10.1126/science.abm6753

Colloidal nanocrystals of metals, semiconductors, and other functional materials can self-assemble into long-range ordered crystalline and quasicrystalline phases, but insulating organic surface ligands prevent the development of collective electronic states in ordered nanocrystal assemblies. We reversibly self-assembled colloidal nanocrystals of gold. platinum, nickel, lead sulfide, and lead selenide with conductive inorganic ligands into supercrystals exhibiting optical and electronic properties consistent with strong electronic coupling between the constituent nanocrystals. The phase behavior of charge-stabilized nanocrystals can be rationalized and navigated with phase diagrams computed for particles interacting through short-range attractive potentials. By finely tuning interparticle interactions, the assembly was directed either through one-step nucleation or nonclassical two-step nucleation pathways. In the latter case, the nucleation was preceded by the formation of two metastable colloidal fluids.

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