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

Handle URI:
http://hdl.handle.net/10754/597867
Title:
Controlling Nanocrystal Superlattice Symmetry and Shape-Anisotropic Interactions through Variable Ligand Surface Coverage
Authors:
Choi, Joshua J.; Bealing, Clive R.; Bian, Kaifu; Hughes, Kevin J.; Zhang, Wenyu; Smilgies, Detlef-M.; Hennig, Richard G.; Engstrom, James R.; Hanrath, Tobias
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.
Citation:
Choi JJ, Bealing CR, Bian K, Hughes KJ, Zhang W, et al. (2011) Controlling Nanocrystal Superlattice Symmetry and Shape-Anisotropic Interactions through Variable Ligand Surface Coverage. Journal of the American Chemical Society 133: 3131–3138. Available: http://dx.doi.org/10.1021/ja110454b.
Publisher:
American Chemical Society (ACS)
Journal:
Journal of the American Chemical Society
KAUST Grant Number:
KUS-C1-018-02
Issue Date:
9-Mar-2011
DOI:
10.1021/ja110454b
PubMed ID:
21306161
Type:
Article
ISSN:
0002-7863; 1520-5126
Sponsors:
This work was supported in part by Award No. KUS-C1-018-02, made by King Abdullah University of Science and Technology (KAUST) and by the National Science Foundation, Award NSF-CBET 0828703. J.J.C. was supported by the NSF IGERT Fellowship Program on "Nanoscale Control of Surfaces and Interfaces," administered by Cornell's MRSEC. K.B. was supported by NSF-CBET 0828703. GISAXS measurements were conducted at the Cornell High Energy Synchrotron Source (CHESS), which is supported by the National Science Foundation and the National Institutes of Health/National Institute of General Medical Sciences under NSF Award DMR-0936384. This research used computational resources of the Computation Center for Nanotechnology Innovation at Rensselaer Polytechnic Institute and was supported in part by the National Science Foundation through TeraGrid computational resources provided by the National Center for Supercomputing Applications, the Texas Advanced Computing Center and under the Louisiana Optical Network Initiative under Grant No. DMR050036
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Full metadata record

DC FieldValue Language
dc.contributor.authorChoi, Joshua J.en
dc.contributor.authorBealing, Clive R.en
dc.contributor.authorBian, Kaifuen
dc.contributor.authorHughes, Kevin J.en
dc.contributor.authorZhang, Wenyuen
dc.contributor.authorSmilgies, Detlef-M.en
dc.contributor.authorHennig, Richard G.en
dc.contributor.authorEngstrom, James R.en
dc.contributor.authorHanrath, Tobiasen
dc.date.accessioned2016-02-25T12:58:04Zen
dc.date.available2016-02-25T12:58:04Zen
dc.date.issued2011-03-09en
dc.identifier.citationChoi JJ, Bealing CR, Bian K, Hughes KJ, Zhang W, et al. (2011) Controlling Nanocrystal Superlattice Symmetry and Shape-Anisotropic Interactions through Variable Ligand Surface Coverage. Journal of the American Chemical Society 133: 3131–3138. Available: http://dx.doi.org/10.1021/ja110454b.en
dc.identifier.issn0002-7863en
dc.identifier.issn1520-5126en
dc.identifier.pmid21306161en
dc.identifier.doi10.1021/ja110454ben
dc.identifier.urihttp://hdl.handle.net/10754/597867en
dc.description.abstractThe 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.en
dc.description.sponsorshipThis work was supported in part by Award No. KUS-C1-018-02, made by King Abdullah University of Science and Technology (KAUST) and by the National Science Foundation, Award NSF-CBET 0828703. J.J.C. was supported by the NSF IGERT Fellowship Program on "Nanoscale Control of Surfaces and Interfaces," administered by Cornell's MRSEC. K.B. was supported by NSF-CBET 0828703. GISAXS measurements were conducted at the Cornell High Energy Synchrotron Source (CHESS), which is supported by the National Science Foundation and the National Institutes of Health/National Institute of General Medical Sciences under NSF Award DMR-0936384. This research used computational resources of the Computation Center for Nanotechnology Innovation at Rensselaer Polytechnic Institute and was supported in part by the National Science Foundation through TeraGrid computational resources provided by the National Center for Supercomputing Applications, the Texas Advanced Computing Center and under the Louisiana Optical Network Initiative under Grant No. DMR050036en
dc.publisherAmerican Chemical Society (ACS)en
dc.titleControlling Nanocrystal Superlattice Symmetry and Shape-Anisotropic Interactions through Variable Ligand Surface Coverageen
dc.typeArticleen
dc.identifier.journalJournal of the American Chemical Societyen
dc.contributor.institutionCornell University, Ithaca, United Statesen
kaust.grant.numberKUS-C1-018-02en

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