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Title: The Role of Repulsion in Colloidal Crystal Engineering with DNA

Abstract

Hybridization interactions between DNA-functionalized nanoparticles (DNA-NPs) can be used to program the crystallization behavior of superlattices, yielding access to complex three-dimensional structures with more than 30 different lattice symmetries. The first superlattice structures using DNA-NPs as building blocks were identified almost two decades ago, yet the role of repulsive interactions in guiding structure formation is still largely unexplored. Here, a com-prehensive approach is taken to study the role of repulsion in the assembly behavior of DNA-NPs, enabling the calculation of interparticle interaction potentials based on experimental results. In this work, we used two different means to assemble DNA-NPs—Watson-Crick base pairing interactions and depletion interactions—and systematically varied the salt concen-tration to study the effective interactions in DNA-NP superlattices. A comparison between the two systems allows us to decouple the repulsive forces from the attractive hybridization interactions that are sensitive to the ionic environment. We find that the gap distance between adjacent DNA-NPs follows a simple power law dependence on solution ionic strength regardless of the type of attractive forces present. This result suggests that the observed trend is driven by repulsive inter-actions. To better understand such behavior, we propose a mean-field model that provides a mathematical description for the observed trend.more » This model shows that the trend is due to the variation in the effective cross-sectional diameter of DNA duplex and the thickness of DNA shell.« less

Authors:
 [1];  [2];  [2]; ORCiD logo [1]; ORCiD logo [2]
  1. Northwestern Univ., Evanston, IL (United States). Dept. of Chemistry. International Inst. for Nanotechnology
  2. Argonne National Lab. (ANL), Argonne, IL (United States). X-ray Science Division
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:
1422594
Alternate Identifier(s):
OSTI ID: 1415591
Grant/Contract Number:  
AC02-06CH11357; SC0000989
Resource Type:
Accepted Manuscript
Journal Name:
Journal of the American Chemical Society
Additional Journal Information:
Journal Volume: 139; Journal Issue: 46; Journal ID: ISSN 0002-7863
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
59 BASIC BIOLOGICAL SCIENCES; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Seo, Soyoung E., Li, Tao, Senesi, Andrew J., Mirkin, Chad A., and Lee, Byeongdu. The Role of Repulsion in Colloidal Crystal Engineering with DNA. United States: N. p., 2017. Web. https://doi.org/10.1021/jacs.7b06734.
Seo, Soyoung E., Li, Tao, Senesi, Andrew J., Mirkin, Chad A., & Lee, Byeongdu. The Role of Repulsion in Colloidal Crystal Engineering with DNA. United States. https://doi.org/10.1021/jacs.7b06734
Seo, Soyoung E., Li, Tao, Senesi, Andrew J., Mirkin, Chad A., and Lee, Byeongdu. Tue . "The Role of Repulsion in Colloidal Crystal Engineering with DNA". United States. https://doi.org/10.1021/jacs.7b06734. https://www.osti.gov/servlets/purl/1422594.
@article{osti_1422594,
title = {The Role of Repulsion in Colloidal Crystal Engineering with DNA},
author = {Seo, Soyoung E. and Li, Tao and Senesi, Andrew J. and Mirkin, Chad A. and Lee, Byeongdu},
abstractNote = {Hybridization interactions between DNA-functionalized nanoparticles (DNA-NPs) can be used to program the crystallization behavior of superlattices, yielding access to complex three-dimensional structures with more than 30 different lattice symmetries. The first superlattice structures using DNA-NPs as building blocks were identified almost two decades ago, yet the role of repulsive interactions in guiding structure formation is still largely unexplored. Here, a com-prehensive approach is taken to study the role of repulsion in the assembly behavior of DNA-NPs, enabling the calculation of interparticle interaction potentials based on experimental results. In this work, we used two different means to assemble DNA-NPs—Watson-Crick base pairing interactions and depletion interactions—and systematically varied the salt concen-tration to study the effective interactions in DNA-NP superlattices. A comparison between the two systems allows us to decouple the repulsive forces from the attractive hybridization interactions that are sensitive to the ionic environment. We find that the gap distance between adjacent DNA-NPs follows a simple power law dependence on solution ionic strength regardless of the type of attractive forces present. This result suggests that the observed trend is driven by repulsive inter-actions. To better understand such behavior, we propose a mean-field model that provides a mathematical description for the observed trend. This model shows that the trend is due to the variation in the effective cross-sectional diameter of DNA duplex and the thickness of DNA shell.},
doi = {10.1021/jacs.7b06734},
journal = {Journal of the American Chemical Society},
number = 46,
volume = 139,
place = {United States},
year = {2017},
month = {10}
}

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