Journal
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
Volume 133, Issue 9, Pages 3131-3138Publisher
AMER CHEMICAL SOC
DOI: 10.1021/ja110454b
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Funding
- King Abdullah University of Science and Technology (KAUST) [KUS-C1-018-02]
- National Science Foundation [NSF-CBET 0828703]
- NSF
- Cornell's MRSEC
- National Institutes of Health/National Institute of General Medical Sciences (NSF) [DMR-0936384]
- National Center for Supercomputing Applications
- Texas Advanced Computing Center
- Louisiana Optical Network Initiative [DMR050036]
- Div Of Chem, Bioeng, Env, & Transp Sys
- Directorate For Engineering [0828703] Funding Source: National Science Foundation
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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.
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