Emergence of hierarchical structural complexities in nanoparticles and their assembly

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Science  23 Dec 2016:
Vol. 354, Issue 6319, pp. 1580-1584
DOI: 10.1126/science.aak9750

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Probing packing rules

The crystals of a well-defined ligand-covered gold nanoparticle can reveal how packing into a lattice happens. Zeng et al. synthesized nanoparticles with a 246-atom gold core surrounded by 80 4-methylbenzenethiol ligands. These nearly spherical nanoparticles did not pack into a cubic arrangement but instead formed a lower-symmetry monoclinic structure. A hierarchy of interparticle ligand interactions controlled the packing, including sets of chiral packing arrangements that reversed between layers.

Science, this issue p. 1580


We demonstrate that nanoparticle self-assembly can reach the same level of hierarchy, complexity, and accuracy as biomolecules. The precise assembly structures of gold nanoparticles (246 gold core atoms with 80 p-methylbenzenethiolate surface ligands) at the atomic, molecular, and nanoscale levels were determined from x-ray diffraction studies. We identified the driving forces and rules that guide the multiscale assembly behavior. The protecting ligands self-organize into rotational and parallel patterns on the nanoparticle surface via C-H⋅⋅⋅π interaction, and the symmetry and density of surface patterns dictate directional packing of nanoparticles into crystals with orientational, rotational, and translational orders. Through hierarchical interactions and symmetry matching, the simple building blocks evolve into complex structures, representing an emergent phenomenon in the nanoparticle system.

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