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

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. Department of Chemistry and International Institute for Nanotechnology, Northwestern University, 2145 Sheridan Road, Evanston, Illinois 60208, United States
  2. X-ray Science Division, Argonne National Laboratory, 9700 Cass Avenue, Lemont, Illinois 60439, United States
Publication Date:
Grant/Contract Number:
AC02-06CH11357; SC0000989
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)
Research Org:
Argonne National Lab. (ANL), Argonne, IL (United States); Energy Frontier Research Centers (EFRC) (United States). Center for Bio-Inspired Energy Science (CBES); Northwestern Univ., Evanston, IL (United States)
Sponsoring Org:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
Country of Publication:
United States
Language:
English
Subject:
59 BASIC BIOLOGICAL SCIENCES; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
OSTI Identifier:
1422594
Alternate Identifier(s):
OSTI ID: 1415591

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., Web. doi: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. doi:10.1021/jacs.7b06734.
Seo, Soyoung E., Li, Tao, Senesi, Andrew J., Mirkin, Chad A., and Lee, Byeongdu. 2017. "The Role of Repulsion in Colloidal Crystal Engineering with DNA". United States. doi: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 = {11}
}