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. These observations provide important insight into how solution ionic strength can be usedmore »
- 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)
- OSTI Identifier:
- 1490106
- Alternate Identifier(s):
- OSTI ID: 1494055; OSTI ID: 1508768
- Grant/Contract Number:
- AC02-06CH11357; SC0000989
- Resource Type:
- Published Article
- Journal Name:
- ACS Central Science
- Additional Journal Information:
- Journal Name: ACS Central Science Journal Volume: 5 Journal Issue: 1; Journal ID: ISSN 2374-7943
- Publisher:
- American Chemical Society
- 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. https://doi.org/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. https://doi.org/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. 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},
number = 1,
volume = 5,
place = {United States},
year = {2019},
month = {1}
}
https://doi.org/10.1021/acscentsci.8b00826
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Figures / Tables:
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 »
Works referencing / citing this record:
DNA‐ and Field‐Mediated Assembly of Magnetic Nanoparticles into High‐Aspect Ratio Crystals
journal, December 2019
- Park, Sarah S.; Urbach, Zachary J.; Brisbois, Chase A.
- Advanced Materials, Vol. 32, Issue 4
Figures / Tables found in this record: