Controlling Nanocrystal Superlattice Symmetry and Shape-Anisotropic Interactions through Variable Ligand Surface Coverage

Joshua J. Choi, Clive R. Bealing, Kaifu Bian, Kevin J. Hughes, Wenyu Zhang, Detlef-M. Smilgies, Richard G. Hennig, James R. Engstrom, Tobias Hanrath

Research output: Contribution to journalArticlepeer-review

159 Scopus citations

Abstract

The assembly of colloidal nanocrystals (NCs) into superstructures with long-range translational and orientational order is sensitive to the molecular interactions between ligands bound to the NC surface. We illustrate how ligand coverage on colloidal PbS NCs can be exploited as a tunable parameter to direct the self-assembly of superlattices with predefined symmetry. We show that PbS NCs with dense ligand coverage assemble into face-centered cubic (fcc) superlattices whereas NCs with sparse ligand coverage assemble into body-centered cubic (bcc) superlattices which also exhibit orientational ordering of NCs in their lattice sites. Surface chemistry characterization combined with density functional theory calculations suggest that the loss of ligands occurs preferentially on {100} than on reconstructed {111} NC facets. The resulting anisotropic ligand distribution amplifies the role of NC shape in the assembly and leads to the formation of superlattices with translational and orientational order. © 2011 American Chemical Society.
Original languageEnglish (US)
Pages (from-to)3131-3138
Number of pages8
JournalJournal of the American Chemical Society
Volume133
Issue number9
DOIs
StatePublished - Mar 9 2011
Externally publishedYes

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