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Title: The Importance of Salt-Enhanced Electrostatic Repulsion in Colloidal Crystal Engineering with DNA

Abstract

Realizing functional colloidal single crystals requires precise control over nanoparticles in three dimensions across multiple size regimes. In this regard, colloidal crystallization with programmable atom equivalents (PAEs) composed of DNA-modified nanoparticles allows one to program in a sequence-specific manner crystal symmetry, lattice parameter, and, in certain cases, crystal habit. Here, we explore how salt and the electrostatic properties of DNA regulate the attachment kinetics between PAEs. Counterintuitively, simulations and theory show that at high salt concentrations (1 M NaCl), the energy barrier for crystal growth increases by over an order of magnitude compared to low concentration (0.3 M), resulting in a transition from interface-limited to diffusion-limited crystal growth at larger crystal sizes. Remarkably, at elevated salt concentrations, well-formed rhombic dodecahedron-shaped microcrystals up to 21 μm in size grow, whereas at low salt concentration, the crystal size typically does not exceed 2 μm. Simulations show an increased barrier to hybridization between complementary PAEs at elevated salt concentrations. Therefore, although one might intuitively conclude that higher salt concentration would lead to less electrostatic repulsion and faster PAE-to-PAE hybridization kinetics, the opposite is the case, especially at larger inter-PAE distances. As a result, these observations provide important insight into how solution ionic strengthmore » can be used to control the attachment kinetics of nanoparticles coated with charged polymeric materials in general and DNA in particular.« less

Authors:
ORCiD logo [1];  [1];  [1]; ORCiD logo [1]
  1. Northwestern Univ., Evanston, IL (United States)
Publication Date:
Research Org.:
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)
OSTI Identifier:
1490106
Alternate Identifier(s):
OSTI ID: 1494055; OSTI ID: 1508768
Grant/Contract Number:  
SC0000989; AC02-06CH11357
Resource Type:
Journal Article: Published Article
Journal Name:
ACS Central Science
Additional Journal Information:
Journal Volume: 5; Journal Issue: 1; Journal ID: ISSN 2374-7943
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Seo, Soyoung E., Girard, Martin, de la Cruz, Monica Olvera, and Mirkin, Chad A. The Importance of Salt-Enhanced Electrostatic Repulsion in Colloidal Crystal Engineering with DNA. United States: N. p., 2019. Web. doi:10.1021/acscentsci.8b00826.
Seo, Soyoung E., Girard, Martin, de la Cruz, Monica Olvera, & Mirkin, Chad A. The Importance of Salt-Enhanced Electrostatic Repulsion in Colloidal Crystal Engineering with DNA. United States. doi:10.1021/acscentsci.8b00826.
Seo, Soyoung E., Girard, Martin, de la Cruz, Monica Olvera, and Mirkin, Chad A. Tue . "The Importance of Salt-Enhanced Electrostatic Repulsion in Colloidal Crystal Engineering with DNA". United States. doi:10.1021/acscentsci.8b00826.
@article{osti_1490106,
title = {The Importance of Salt-Enhanced Electrostatic Repulsion in Colloidal Crystal Engineering with DNA},
author = {Seo, Soyoung E. and Girard, Martin and de la Cruz, Monica Olvera and Mirkin, Chad A.},
abstractNote = {Realizing functional colloidal single crystals requires precise control over nanoparticles in three dimensions across multiple size regimes. In this regard, colloidal crystallization with programmable atom equivalents (PAEs) composed of DNA-modified nanoparticles allows one to program in a sequence-specific manner crystal symmetry, lattice parameter, and, in certain cases, crystal habit. Here, we explore how salt and the electrostatic properties of DNA regulate the attachment kinetics between PAEs. Counterintuitively, simulations and theory show that at high salt concentrations (1 M NaCl), the energy barrier for crystal growth increases by over an order of magnitude compared to low concentration (0.3 M), resulting in a transition from interface-limited to diffusion-limited crystal growth at larger crystal sizes. Remarkably, at elevated salt concentrations, well-formed rhombic dodecahedron-shaped microcrystals up to 21 μm in size grow, whereas at low salt concentration, the crystal size typically does not exceed 2 μm. Simulations show an increased barrier to hybridization between complementary PAEs at elevated salt concentrations. Therefore, although one might intuitively conclude that higher salt concentration would lead to less electrostatic repulsion and faster PAE-to-PAE hybridization kinetics, the opposite is the case, especially at larger inter-PAE distances. As a result, these observations provide important insight into how solution ionic strength can be used to control the attachment kinetics of nanoparticles coated with charged polymeric materials in general and DNA in particular.},
doi = {10.1021/acscentsci.8b00826},
journal = {ACS Central Science},
issn = {2374-7943},
number = 1,
volume = 5,
place = {United States},
year = {2019},
month = {1}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record at 10.1021/acscentsci.8b00826

Citation Metrics:
Cited by: 1 work
Citation information provided by
Web of Science

Figures / Tables:

Figure 1 Figure 1: (A) A snapshot of two complementary PAEs at different salt concentrations in simulations. The centers of the 15 nm nanoparticles are 370 Å apart in this snapshot. (B) Pair potential energies between complementary PAEs were calculated across a range of interparticle distances. PAEs exhibit a well-defined equilibrium interparticlemore » distance at potential minimum. At an interparticle distance of 380 Å, the attachment barrier peaks; this increases with increasing salt concentration. (C) Mean crystal size obtained without coarsening as a function of the attachment rate to the surface.« less

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