Self-organization of Electrostatically and Sterically Stabilized Colloidal Nanocrystals: The Roles of Topology, Image Charges and Non-classical Nucleation
Dmitri Talapin a
a Department of Chemistry, University of Chicago, Chicago, Illinois 60637, USA
nanoGe Fall Meeting
Proceedings of nanoGe Fall Meeting19 (NGFM19)
#NCFun19. Fundamental Processes in Semiconductor Nanocrystals
Berlin, Germany, 2019 November 3rd - 8th
Organizers: Ivan Infante, Matthew Mayer, Ludmilla Steier, Jörg Ackermann, Claudine Katan, Jonathan Owen, Wolfgang Tress, Uli Würfel and Simone Meloni
Keynote, Dmitri Talapin, presentation 297
Publication date: 16th July 2019

Colloidal nanocrystals offer a route toward engineering new classes of materials by acting as discrete units that can be assembled to construct composite solids. The self-assembly of two sizes of spherical nanocrystals has revealed a surprisingly diverse library of structures. To date, at least fifteen distinct binary nanocrystal superlattice (BNSL) structures have been documented. BNSLs naturally represent a powerful platform for practical implementations of multifunctional materials. However, the stability of the observed binary phases cannot be fully explained using the traditional conceptual framework treating the assembly process as entropy-driven crystallization of rigid spherical particles. We evaluate new theoretical models treating the co-crystallization of deformable spheres and to formulate new hypotheses about the factors affecting the nucleation and growth of the binary superlattices. The deviation from hard sphere behavior can be explained by specific topological textures developed within deformable layers of surface ligands. Our results also suggest that the relative abundance of BNSL phases is determined not only by their thermodynamic phase stability but also by a postulated pre-ordering of the binary fluid into local structures with icosahedral or polytetrahedral structures prior to nucleation.

Strong electronic coupling between individual nanocrystals within a superlattice is an important prerequisite for the emergence of non-additive physical properties. However, a simultaneous realization of strong electronic coupling and dense ordered packing of nanocrystal solids has remained elusive. We report a method for growing all-inorganic highly ordered solids of electrostatically-stabilized nanocrystals with the interstitial space filled with a glassy metal chalcogenide matrix which, combined with the short separation between particles leads to very strong electronic coupling. Temperature-dependent conductivity measurements show metallic transport across our supercrystals. The formation of strongly-coupled all-inorganic nanocrystal assemblies represents an important step toward the bottom-up design of functional nanostructured composites.

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