Dendrimer Ligand Directed Nanoplate Assembly

Elbert, Katherine C.; Vo, Thi; Krook, Nadia M.; Zygmunt, William; Park, Jungmi; Yager, Kevin G.; Composto, Russell J.; Glotzer, Sharon C.; Murray, Christopher B.

doi:10.1021/acsnano.9b07348

Title: Dendrimer Ligand Directed Nanoplate Assembly

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Abstract

Many studies on nanocrystal (NC) self-assembly into ordered superlattices have focused mainly on attractive forces between the NCs, whereas the role of organic ligands on anisotropic NCs is only in its infancy. Herein, we report the use of a series of dendrimer ligands to direct the assembly of nanoplates into 2D and 3D geometries. It was found that the dendrimer-nanoplates consistently form a directionally offset architecture in 3D films. We present a theory to predict ligand surface distribution and Monte Carlo simulation results that characterize the ligand shell around the nanoplates. Bulky dendrimer ligands create a nontrivial corona around the plates that changes with ligand architecture. When this organic–inorganic effective shape is used in conjunction with thermodynamic perturbation theory to predict both lattice morphology and equilibrium relative orientations between NCs, a lock-and-key type of mechanism is found for the 3D assembly. We observe excellent agreement between our experimental results and theoretical model for 2D and 3D geometries, including the percent of offset between the layers of NCs. Furthermore, such level of theoretical understanding and modeling will help guide future design frameworks to achieve targeted assemblies of NCs

Authors:

^[1]; Vo, Thi ^[2];

^[1]; Zygmunt, William ^[2]; Park, Jungmi ^[1];

^[3];

^[1]; Glotzer, Sharon C. ^[2]; Murray, Christopher B. ^[1]

Univ. of Pennsylvania, Philadelphia, PA (United States)
Univ. of Michigan, Ann Arbor, MI (United States)
Brookhaven National Lab. (BNL), Upton, NY (United States). Center for Functional Nanomaterials (CFN)

Publication Date:: Fri Nov 22 00:00:00 EST 2019

Research Org.:: Brookhaven National Lab. (BNL), Upton, NY (United States)

Sponsoring Org.:: US Department of the Navy, Office of Naval Research (ONR); National Science Foundation (NSF); US Air Force Office of Scientific Research (AFOSR); USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities Division

OSTI Identifier:: 1599291

Report Number(s):: BNL-213620-2020-JAAM
Journal ID: ISSN 1936-0851

Grant/Contract Number:: SC0012704; ONR N00014-18-1-2497; DGE-1321851; FA9550-11-C-0028; ACI-1053575; DMR 140129; POLYMERS-DMR-1507713; POLYMERS-DMR-1905912; PIRE-OISE-1545884; MRSEC-DMR-1720530

Resource Type:: Accepted Manuscript

Journal Name:: ACS Nano

Additional Journal Information:: Journal Volume: 13; Journal Issue: 12; Journal ID: ISSN 1936-0851

Publisher:: American Chemical Society (ACS)

Country of Publication:: United States

Language:: English

Subject:: 77 NANOSCIENCE AND NANOTECHNOLOGY; Thin films; Ligands; Layers; Nanoparticles; Mathematical methods

Citation Formats


                    Elbert, Katherine C., Vo, Thi, Krook, Nadia M., Zygmunt, William, Park, Jungmi, Yager, Kevin G., Composto, Russell J., Glotzer, Sharon C., and Murray, Christopher B. Dendrimer Ligand Directed Nanoplate Assembly.  United States: N. p., 2019. 
Web.  doi:10.1021/acsnano.9b07348.

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                    Elbert, Katherine C., Vo, Thi, Krook, Nadia M., Zygmunt, William, Park, Jungmi, Yager, Kevin G., Composto, Russell J., Glotzer, Sharon C., & Murray, Christopher B. Dendrimer Ligand Directed Nanoplate Assembly.  United States.  https://doi.org/10.1021/acsnano.9b07348

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                    Elbert, Katherine C., Vo, Thi, Krook, Nadia M., Zygmunt, William, Park, Jungmi, Yager, Kevin G., Composto, Russell J., Glotzer, Sharon C., and Murray, Christopher B. Fri .  
"Dendrimer Ligand Directed Nanoplate Assembly".  United States.  https://doi.org/10.1021/acsnano.9b07348.  https://www.osti.gov/servlets/purl/1599291.

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@article{osti_1599291,

  title        = {Dendrimer Ligand Directed Nanoplate Assembly},

  author       = {Elbert, Katherine C. and Vo, Thi and Krook, Nadia M. and Zygmunt, William and Park, Jungmi and Yager, Kevin G. and Composto, Russell J. and Glotzer, Sharon C. and Murray, Christopher B.},

  abstractNote = {Many studies on nanocrystal (NC) self-assembly into ordered superlattices have focused mainly on attractive forces between the NCs, whereas the role of organic ligands on anisotropic NCs is only in its infancy. Herein, we report the use of a series of dendrimer ligands to direct the assembly of nanoplates into 2D and 3D geometries. It was found that the dendrimer-nanoplates consistently form a directionally offset architecture in 3D films. We present a theory to predict ligand surface distribution and Monte Carlo simulation results that characterize the ligand shell around the nanoplates. Bulky dendrimer ligands create a nontrivial corona around the plates that changes with ligand architecture. When this organic–inorganic effective shape is used in conjunction with thermodynamic perturbation theory to predict both lattice morphology and equilibrium relative orientations between NCs, a lock-and-key type of mechanism is found for the 3D assembly. We observe excellent agreement between our experimental results and theoretical model for 2D and 3D geometries, including the percent of offset between the layers of NCs. Furthermore, such level of theoretical understanding and modeling will help guide future design frameworks to achieve targeted assemblies of NCs},

  doi          = {10.1021/acsnano.9b07348},

  journal      = {ACS Nano},

  number       = 12,

  volume       = 13,

  place        = {United States},

  year         = {Fri Nov 22 00:00:00 EST 2019},

  month        = {Fri Nov 22 00:00:00 EST 2019}

}

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