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Title: Unusual packing of soft-shelled nanocubes

Abstract

Space-filling generally governs hard particle packing and the resulting phases and interparticle orientations. Contrastingly, hard-shaped nanoparticles with grafted soft-ligands pack differently since the energetically interacting soft-shell is amenable to nanoscale sculpturing. While the interplay between the shape and soft-shell can lead to unforeseen packing effects, little is known about the underlying physics. Here, using electron microscopy and small-angle x-ray scattering, we demonstrate that nanoscale cubes with soft, grafted DNA shells exhibit remarkable packing, distinguished by orientational symmetry breaking of cubes relative to the unit cell vectors. This zigzag arrangement occurs in flat body-centered tetragonal and body-centered cubic phases. We ascribe this unique arrangement to the interplay between shape and a spatially anisotropic shell resulting from preferential grafting of ligands to regions of high curvature. These observations reveal the decisive role played by shell-modulated anisotropy in nanoscale packing and suggest a plethora of new spatial organizations for molecularly decorated shaped nanoparticles.

Authors:
ORCiD logo [1];  [2]; ORCiD logo [1]; ORCiD logo [2]; ORCiD logo [1];  [2]; ORCiD logo [3]
  1. Brookhaven National Lab. (BNL), Upton, NY (United States)
  2. Columbia Univ., New York, NY (United States)
  3. Brookhaven National Lab. (BNL), Upton, NY (United States); Columbia Univ., New York, NY (United States)
Publication Date:
Research Org.:
Brookhaven National Lab. (BNL), Upton, NY (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1569014
Report Number(s):
BNL-212167-2019-JAAM
Journal ID: ISSN 2375-2548
Grant/Contract Number:  
SC0012704; SC0008772
Resource Type:
Accepted Manuscript
Journal Name:
Science Advances
Additional Journal Information:
Journal Volume: 5; Journal Issue: 5; Journal ID: ISSN 2375-2548
Publisher:
AAAS
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; 71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSICS

Citation Formats

Lu, Fang, Vo, Thi, Zhang, Yugang, Frenkel, Alex, Yager, Kevin G., Kumar, Sanat, and Gang, Oleg. Unusual packing of soft-shelled nanocubes. United States: N. p., 2019. Web. doi:10.1126/sciadv.aaw2399.
Lu, Fang, Vo, Thi, Zhang, Yugang, Frenkel, Alex, Yager, Kevin G., Kumar, Sanat, & Gang, Oleg. Unusual packing of soft-shelled nanocubes. United States. doi:10.1126/sciadv.aaw2399.
Lu, Fang, Vo, Thi, Zhang, Yugang, Frenkel, Alex, Yager, Kevin G., Kumar, Sanat, and Gang, Oleg. Fri . "Unusual packing of soft-shelled nanocubes". United States. doi:10.1126/sciadv.aaw2399. https://www.osti.gov/servlets/purl/1569014.
@article{osti_1569014,
title = {Unusual packing of soft-shelled nanocubes},
author = {Lu, Fang and Vo, Thi and Zhang, Yugang and Frenkel, Alex and Yager, Kevin G. and Kumar, Sanat and Gang, Oleg},
abstractNote = {Space-filling generally governs hard particle packing and the resulting phases and interparticle orientations. Contrastingly, hard-shaped nanoparticles with grafted soft-ligands pack differently since the energetically interacting soft-shell is amenable to nanoscale sculpturing. While the interplay between the shape and soft-shell can lead to unforeseen packing effects, little is known about the underlying physics. Here, using electron microscopy and small-angle x-ray scattering, we demonstrate that nanoscale cubes with soft, grafted DNA shells exhibit remarkable packing, distinguished by orientational symmetry breaking of cubes relative to the unit cell vectors. This zigzag arrangement occurs in flat body-centered tetragonal and body-centered cubic phases. We ascribe this unique arrangement to the interplay between shape and a spatially anisotropic shell resulting from preferential grafting of ligands to regions of high curvature. These observations reveal the decisive role played by shell-modulated anisotropy in nanoscale packing and suggest a plethora of new spatial organizations for molecularly decorated shaped nanoparticles.},
doi = {10.1126/sciadv.aaw2399},
journal = {Science Advances},
number = 5,
volume = 5,
place = {United States},
year = {2019},
month = {5}
}

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Works referenced in this record:

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