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Title: Many Body Effects and Icosahedral Order in Superlattice Self-Assembly

Abstract

Here, we elucidate how nanocrystals “bond” to form ordered structures. For that purpose we consider nanocrystal configurations consisting of regular polygons and polyhedra, which are the motifs that constitute single component and binary nanocrystal superlattices, and simulate them using united atom models. We compute the free energy and quantify many body effects, i.e., those that cannot be accounted for by pair potential (two-body) interactions, further showing that they arise from coalescing vortices of capping ligands. We find that such vortex textures exist for configurations with local coordination number ≤6. For higher coordination numbers, vortices are expelled and nanocrystals arrange in configurations with tetrahedral or icosahedral order. We provide explicit formulas for the optimal separations between nanocrystals, which correspond to the minima of the free energies. Our results quantitatively explain the structure of superlattice nanocrystals as reported in experiments and reveal how packing arguments, extended to include soft components, predict ordered nanocrystal aggregation.

Authors:
ORCiD logo [1];  [1]; ORCiD logo [1]; ORCiD logo [1]
  1. Iowa State Univ. and Ames Lab., Ames, IA (United States)
Publication Date:
Research Org.:
Ames Lab., Ames, IA (United States)
Sponsoring Org.:
USDOE
OSTI Identifier:
1483412
Report Number(s):
IS-J-9694
Journal ID: ISSN 0002-7863
Grant/Contract Number:  
AC02-07CH11358
Resource Type:
Accepted Manuscript
Journal Name:
Journal of the American Chemical Society
Additional Journal Information:
Journal Volume: 140; Journal Issue: 26; Journal ID: ISSN 0002-7863
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSICS

Citation Formats

Waltmann, Tommy, Waltmann, Curt, Horst, Nathan, and Travesset, Alex. Many Body Effects and Icosahedral Order in Superlattice Self-Assembly. United States: N. p., 2018. Web. doi:10.1021/jacs.8b03895.
Waltmann, Tommy, Waltmann, Curt, Horst, Nathan, & Travesset, Alex. Many Body Effects and Icosahedral Order in Superlattice Self-Assembly. United States. doi:10.1021/jacs.8b03895.
Waltmann, Tommy, Waltmann, Curt, Horst, Nathan, and Travesset, Alex. Fri . "Many Body Effects and Icosahedral Order in Superlattice Self-Assembly". United States. doi:10.1021/jacs.8b03895. https://www.osti.gov/servlets/purl/1483412.
@article{osti_1483412,
title = {Many Body Effects and Icosahedral Order in Superlattice Self-Assembly},
author = {Waltmann, Tommy and Waltmann, Curt and Horst, Nathan and Travesset, Alex},
abstractNote = {Here, we elucidate how nanocrystals “bond” to form ordered structures. For that purpose we consider nanocrystal configurations consisting of regular polygons and polyhedra, which are the motifs that constitute single component and binary nanocrystal superlattices, and simulate them using united atom models. We compute the free energy and quantify many body effects, i.e., those that cannot be accounted for by pair potential (two-body) interactions, further showing that they arise from coalescing vortices of capping ligands. We find that such vortex textures exist for configurations with local coordination number ≤6. For higher coordination numbers, vortices are expelled and nanocrystals arrange in configurations with tetrahedral or icosahedral order. We provide explicit formulas for the optimal separations between nanocrystals, which correspond to the minima of the free energies. Our results quantitatively explain the structure of superlattice nanocrystals as reported in experiments and reveal how packing arguments, extended to include soft components, predict ordered nanocrystal aggregation.},
doi = {10.1021/jacs.8b03895},
journal = {Journal of the American Chemical Society},
number = 26,
volume = 140,
place = {United States},
year = {2018},
month = {6}
}

Journal Article:
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Cited by: 12 works
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Figures / Tables:

Figure 1 Figure 1: One of our typical systems with center and cage NCs labeled.

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Works referencing / citing this record:

The Mott to Kondo transition in diluted Kondo superlattices
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Moiré and honeycomb lattices through self-assembly of hard-core/soft-shell microgels: experiment and simulation
journal, January 2019

  • Volk, Kirsten; Deißenbeck, Florian; Mandal, Suvendu
  • Physical Chemistry Chemical Physics, Vol. 21, Issue 35
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Assembly by solvent evaporation: equilibrium structures and relaxation times
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Potential of mean force for two nanocrystals: Core geometry and size, hydrocarbon unsaturation, and universality with respect to the force field
journal, July 2018

  • Waltmann, Curt; Horst, Nathan; Travesset, Alex
  • The Journal of Chemical Physics, Vol. 149, Issue 3
  • DOI: 10.1063/1.5039495

Molecular interaction between asymmetric ligand-capped gold nanocrystals
journal, January 2019

  • Liu, Xuepeng; Lu, Pin; Zhai, Hua
  • The Journal of Chemical Physics, Vol. 150, Issue 3
  • DOI: 10.1063/1.5065476