Structural Diversity in Dimension-Controlled Assemblies of Tetrahedral Gold Nanocrystals.

J Am Chem Soc

Department of Chemistry, Indiana University, Bloomington, Indiana 47405, United States.

Published: August 2022

AI Article Synopsis

  • Polyhedron packings, particularly synthetic tetrahedra, have been a long-standing area of fascination, but their phase behaviors are not yet fully understood due to limited available materials.
  • This study showcases the complex formations achievable with gold nanotetrahedra, where scientists manipulate nanocrystal interactions through surface modifications and assembly conditions to create various two- and three-dimensional structures.
  • The findings present a new methodology for designing superstructures using tetrahedral blocks, which may lead to advancements in the self-assembly and phase behavior studies of colloidal particles.

Article Abstract

Polyhedron packings have fascinated humans for centuries and continue to inspire scientists of modern disciplines. Despite extensive computer simulations and a handful of experimental investigations, understanding of the phase behaviors of synthetic tetrahedra has remained fragmentary largely due to the lack of tetrahedral building blocks with tunable size and versatile surface chemistry. Here, we report the remarkable richness of and complexity in dimension-controlled assemblies of gold nanotetrahedra. By tailoring nanocrystal interactions from long-range repulsive to hard-particle-like or to systems with short-ranged directional attractions through control of surface ligands and assembly conditions, nearly a dozen of two-dimensional and three-dimensional superstructures including the cubic diamond and hexagonal diamond polymorphs are selectively assembled. We further demonstrate multiply twinned icosahedral supracrystals by drying aqueous gold nanotetrahedra on a hydrophobic substrate. This study expands the toolbox of the superstructure by design using tetrahedral building blocks and could spur future computational and experimental work on self-assembly and phase behavior of anisotropic colloidal particles with tunable interactions.

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http://dx.doi.org/10.1021/jacs.2c03196DOI Listing

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