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Title: Controlled Symmetry Breaking in Colloidal Crystal Engineering with DNA

Abstract

The programmed crystallization of particles into low-symmetry lattices represents a major synthetic challenge in the field of colloidal crystal engineering. Herein, we report an approach to realizing such structures that relies on a library of low-symmetry Au nanoparticles, with synthetically adjustable dimensions and tunable aspect ratios. When modified with DNA ligands and used as building blocks for colloidal crystal engineering, these structures enable one to expand the types of accessible lattices and to answer mechanistic questions about phase transitions that break crystal symmetry. Indeed, crystals formed from a library of elongated rhombic dodecahedra yield a rich phase space, including low-symmetry lattices (body-centered tetragonal and hexagonal planar). Molecular dynamics simulations corroborate and insight into the origin of these phase transitions. In particular, we identify an unexpected asymmetry in the DNA shell, distinct from both the particle and lattice symmetries, which enables directional, nonclose-packed interactions.

Authors:
; ORCiD logo; ; ; ; ORCiD logo [1]; ; ORCiD logo
  1. X-Ray Science Division, Argonne National Laboratory, Argonne, Illinois 60439, United States
Publication Date:
Research Org.:
Energy Frontier Research Centers (EFRC) (United States). Center for Bio-Inspired Energy Science (CBES); Argonne National Lab. (ANL), Argonne, IL (United States); Northwestern Univ., Evanston, IL (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1488874
Alternate Identifier(s):
OSTI ID: 1504425; OSTI ID: 1508827
Grant/Contract Number:  
SC0000989; AC02-06CH11357
Resource Type:
Published Article
Journal Name:
ACS Nano
Additional Journal Information:
Journal Name: ACS Nano; Journal ID: ISSN 1936-0851
Publisher:
American Chemical Society
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 36 MATERIALS SCIENCE; Au nanoparticle; DNA; anisotropy; colloidal crystal engineering; symmetry breaking

Citation Formats

Laramy, Christine R., Lopez-Rios, Hector, O’Brien, Matthew N., Girard, Martin, Stawicki, Robert J., Lee, Byeongdu, de la Cruz, Monica Olvera, and Mirkin, Chad A. Controlled Symmetry Breaking in Colloidal Crystal Engineering with DNA. United States: N. p., 2018. Web. doi:10.1021/acsnano.8b07027.
Laramy, Christine R., Lopez-Rios, Hector, O’Brien, Matthew N., Girard, Martin, Stawicki, Robert J., Lee, Byeongdu, de la Cruz, Monica Olvera, & Mirkin, Chad A. Controlled Symmetry Breaking in Colloidal Crystal Engineering with DNA. United States. https://doi.org/10.1021/acsnano.8b07027
Laramy, Christine R., Lopez-Rios, Hector, O’Brien, Matthew N., Girard, Martin, Stawicki, Robert J., Lee, Byeongdu, de la Cruz, Monica Olvera, and Mirkin, Chad A. Wed . "Controlled Symmetry Breaking in Colloidal Crystal Engineering with DNA". United States. https://doi.org/10.1021/acsnano.8b07027.
@article{osti_1488874,
title = {Controlled Symmetry Breaking in Colloidal Crystal Engineering with DNA},
author = {Laramy, Christine R. and Lopez-Rios, Hector and O’Brien, Matthew N. and Girard, Martin and Stawicki, Robert J. and Lee, Byeongdu and de la Cruz, Monica Olvera and Mirkin, Chad A.},
abstractNote = {The programmed crystallization of particles into low-symmetry lattices represents a major synthetic challenge in the field of colloidal crystal engineering. Herein, we report an approach to realizing such structures that relies on a library of low-symmetry Au nanoparticles, with synthetically adjustable dimensions and tunable aspect ratios. When modified with DNA ligands and used as building blocks for colloidal crystal engineering, these structures enable one to expand the types of accessible lattices and to answer mechanistic questions about phase transitions that break crystal symmetry. Indeed, crystals formed from a library of elongated rhombic dodecahedra yield a rich phase space, including low-symmetry lattices (body-centered tetragonal and hexagonal planar). Molecular dynamics simulations corroborate and insight into the origin of these phase transitions. In particular, we identify an unexpected asymmetry in the DNA shell, distinct from both the particle and lattice symmetries, which enables directional, nonclose-packed interactions.},
doi = {10.1021/acsnano.8b07027},
journal = {ACS Nano},
number = ,
volume = ,
place = {United States},
year = {Wed Dec 26 00:00:00 EST 2018},
month = {Wed Dec 26 00:00:00 EST 2018}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record
https://doi.org/10.1021/acsnano.8b07027

Citation Metrics:
Cited by: 14 works
Citation information provided by
Web of Science

Figures / Tables:

Figure 1 Figure 1: A rod-based seed-mediated synthesis can be used to generate elongated rhombic dodecahedra with tunable ARs. (a) Schematics show a seed-mediated synthesis with a sphere or a rod seed and their resultant products. Green indicates an elongated side facet, and purple indicates a tip facet. (b) Seed AR andmore » different [seed]:[Au3+] ratios can be used to tune product AR. The algorithmic analysis of several hundred nanoparticles per sample from transmission electron microscopy (TEM) images can be used to quantitate this relationship. (c) Representative TEM images show seed and product particles that correspond to the colors in the plot in (b). The scale bar represents 100 nm.« less

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Works referencing / citing this record:

Crystal engineering with DNA
journal, February 2019

  • Laramy, Christine R.; O’Brien, Matthew N.; Mirkin, Chad A.
  • Nature Reviews Materials, Vol. 4, Issue 3
  • DOI: 10.1038/s41578-019-0087-2

Novel assemblies based on oligonucleotides containing intercalating nucleic acid monomers
journal, November 2019

  • Abdelrahman, Asmaa; Gouda, Alaa S.; Jørgensen, Per T.
  • Nucleosides, Nucleotides & Nucleic Acids, Vol. 39, Issue 1-3
  • DOI: 10.1080/15257770.2019.1683188

Figures/Tables have been extracted from DOE-funded journal article accepted manuscripts.