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

doi:10.1021/ja110454b

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 journal › Article › peer-review

202 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 language	English (US)
Pages (from-to)	3131-3138
Number of pages	8
Journal	Journal of the American Chemical Society
Volume	133
Issue number	9
DOIs	https://doi.org/10.1021/ja110454b
State	Published - Mar 9 2011
Externally published	Yes

Bibliographical note

KAUST Repository Item: Exported on 2020-10-01
Acknowledged KAUST grant number(s): KUS-C1-018-02
Acknowledgements: 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
This publication acknowledges KAUST support, but has no KAUST affiliated authors.

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@article{a22ef3f187394988a79647c40c9f9051,

title = "Controlling Nanocrystal Superlattice Symmetry and Shape-Anisotropic Interactions through Variable Ligand Surface Coverage",

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. {\textcopyright} 2011 American Chemical Society.",

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

note = "KAUST Repository Item: Exported on 2020-10-01 Acknowledged KAUST grant number(s): KUS-C1-018-02 Acknowledgements: 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 This publication acknowledges KAUST support, but has no KAUST affiliated authors.",

year = "2011",

month = mar,

day = "9",

doi = "10.1021/ja110454b",

language = "English (US)",

volume = "133",

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T1 - Controlling Nanocrystal Superlattice Symmetry and Shape-Anisotropic Interactions through Variable Ligand Surface Coverage

AU - Choi, Joshua J.

AU - Bealing, Clive R.

AU - Bian, Kaifu

AU - Hughes, Kevin J.

AU - Zhang, Wenyu

AU - Smilgies, Detlef-M.

AU - Hennig, Richard G.

AU - Engstrom, James R.

AU - Hanrath, Tobias

N1 - KAUST Repository Item: Exported on 2020-10-01 Acknowledged KAUST grant number(s): KUS-C1-018-02 Acknowledgements: 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 This publication acknowledges KAUST support, but has no KAUST affiliated authors.

PY - 2011/3/9

Y1 - 2011/3/9

N2 - 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.

AB - 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.

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UR - https://pubs.acs.org/doi/10.1021/ja110454b

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DO - 10.1021/ja110454b

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C2 - 21306161

SN - 0002-7863

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EP - 3138

JO - Journal of the American Chemical Society

JF - Journal of the American Chemical Society

IS - 9

ER -

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

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