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Title: Altering DNA-Programmable Colloidal Crystallization Paths by Modulating Particle Repulsion

Abstract

Colloidal crystal engineering with DNA can be used to realize precise control over nanoparticle (NP) arrangement. Here, we investigate a case of DNA-based assembly where the properties of DNA as a polyelectrolyte brush are employed to alter a hybridization-driven NP crystallization pathway. Using the co-assembly of DNA-conjugated proteins and spherical gold 2 nanoparticles (AuNPs) as a model system, we explore how steric repulsion between non-complementary, neighboring DNA-NPs due to overlapping DNA shells can influence their ligand-directed behavior. Specifically, our experimental data coupled with coarse-grained molecular dynamics (MD) simulations reveal that by changing factors related to NP repulsion, two structurally distinct outcomes can be achieved. When steric repulsion between DNA-AuNPs is significantly greater than that between DNA-proteins, a lower packing density crystal lattice is favored over the structure that is predicted by design rules based on DNA-hybridization considerations alone. This is enabled by the large difference in DNA density on AuNPs versus proteins and can be tuned by modulating the flexibility, and thus conformational entropy, of the DNA on the constituent particles. At intermediate ligand flexibility, the crystallization pathways are energetically similar and the structural outcome can be adjusted using the density of DNA duplexes on DNA-AuNPs and by screening themore » Coulomb potential between them. Such lattices are shown to undergo dynamic reorganization upon changing salt concentration. These data help elucidate the structural considerations necessary for understanding repulsive forces in DNA-assembly and lay the groundwork for using them to increase architectural diversity in engineering colloidal crystals.« less

Authors:
; ; ; ; ; ; ORCiD logo [1]; ORCiD logo
  1. X-Ray Science Division, Argonne National Laboratory, 9700 S. Cass Avenue, Argonne, Illinois 60439, United States
Publication Date:
Research Org.:
Argonne National Lab. (ANL), Argonne, IL (United States); Energy Frontier Research Centers (EFRC) (United States). Center for Bio-Inspired Energy Science (CBES)
Sponsoring Org.:
US Department of the Navy, Office of Naval Research (ONR); Air Force Research Laboratory (AFRL) - Air Force Office of Scientific Research (AFOSR); USDOE Office of Science - Energy Frontier Research Center - Center for Bio-Inspired Energy Science (CBES); USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22); National Science Foundation (NSF); Natural Sciences and Engineering Research Council of Canada (NSERC)
OSTI Identifier:
1395868
DOE Contract Number:  
AC02-06CH11357
Resource Type:
Journal Article
Journal Name:
Nano Letters
Additional Journal Information:
Journal Volume: 17; Journal Issue: 8; Journal ID: ISSN 1530-6984
Publisher:
American Chemical Society
Country of Publication:
United States
Language:
English
Subject:
DNA; colloidal crystals; nanomaterials; nanoparticle superlattice; protein assembly; self-assembly

Citation Formats

Wang, Mary X., Brodin, Jeffrey D., Millan, Jaime A., Seo, Soyoung E., Girard, Martin, Olvera de la Cruz, Monica, Lee, Byeongdu, and Mirkin, Chad A. Altering DNA-Programmable Colloidal Crystallization Paths by Modulating Particle Repulsion. United States: N. p., 2017. Web. doi:10.1021/acs.nanolett.7b02502.
Wang, Mary X., Brodin, Jeffrey D., Millan, Jaime A., Seo, Soyoung E., Girard, Martin, Olvera de la Cruz, Monica, Lee, Byeongdu, & Mirkin, Chad A. Altering DNA-Programmable Colloidal Crystallization Paths by Modulating Particle Repulsion. United States. doi:10.1021/acs.nanolett.7b02502.
Wang, Mary X., Brodin, Jeffrey D., Millan, Jaime A., Seo, Soyoung E., Girard, Martin, Olvera de la Cruz, Monica, Lee, Byeongdu, and Mirkin, Chad A. Fri . "Altering DNA-Programmable Colloidal Crystallization Paths by Modulating Particle Repulsion". United States. doi:10.1021/acs.nanolett.7b02502.
@article{osti_1395868,
title = {Altering DNA-Programmable Colloidal Crystallization Paths by Modulating Particle Repulsion},
author = {Wang, Mary X. and Brodin, Jeffrey D. and Millan, Jaime A. and Seo, Soyoung E. and Girard, Martin and Olvera de la Cruz, Monica and Lee, Byeongdu and Mirkin, Chad A.},
abstractNote = {Colloidal crystal engineering with DNA can be used to realize precise control over nanoparticle (NP) arrangement. Here, we investigate a case of DNA-based assembly where the properties of DNA as a polyelectrolyte brush are employed to alter a hybridization-driven NP crystallization pathway. Using the co-assembly of DNA-conjugated proteins and spherical gold 2 nanoparticles (AuNPs) as a model system, we explore how steric repulsion between non-complementary, neighboring DNA-NPs due to overlapping DNA shells can influence their ligand-directed behavior. Specifically, our experimental data coupled with coarse-grained molecular dynamics (MD) simulations reveal that by changing factors related to NP repulsion, two structurally distinct outcomes can be achieved. When steric repulsion between DNA-AuNPs is significantly greater than that between DNA-proteins, a lower packing density crystal lattice is favored over the structure that is predicted by design rules based on DNA-hybridization considerations alone. This is enabled by the large difference in DNA density on AuNPs versus proteins and can be tuned by modulating the flexibility, and thus conformational entropy, of the DNA on the constituent particles. At intermediate ligand flexibility, the crystallization pathways are energetically similar and the structural outcome can be adjusted using the density of DNA duplexes on DNA-AuNPs and by screening the Coulomb potential between them. Such lattices are shown to undergo dynamic reorganization upon changing salt concentration. These data help elucidate the structural considerations necessary for understanding repulsive forces in DNA-assembly and lay the groundwork for using them to increase architectural diversity in engineering colloidal crystals.},
doi = {10.1021/acs.nanolett.7b02502},
journal = {Nano Letters},
issn = {1530-6984},
number = 8,
volume = 17,
place = {United States},
year = {2017},
month = {7}
}

Works referencing / citing this record:

Kernel Homology in Gold Nanoclusters
journal, October 2018

  • Zhuang, Shengli; Liao, Lingwen; Yuan, Jinyun
  • Angewandte Chemie International Edition, Vol. 57, Issue 47
  • DOI: 10.1002/anie.201808997