The Role of Repulsion in Colloidal Crystal Engineering with DNA

Seo, Soyoung E.; Li, Tao; Senesi, Andrew J.; Mirkin, Chad A.; Lee, Byeongdu

doi:10.1021/jacs.7b06734

The Role of Repulsion in Colloidal Crystal Engineering with DNA

Journal Article · Mon Nov 06 23:00:00 EST 2017 · Journal of the American Chemical Society

DOI:https://doi.org/10.1021/jacs.7b06734· OSTI ID:1415591

Seo, Soyoung E. ^[1]; Li, Tao ^[2]; Senesi, Andrew J. ^[2]; ^[1]; ^[2]

Department of Chemistry and International Institute for Nanotechnology, Northwestern University, 2145 Sheridan Road, Evanston, Illinois 60208, United States
X-ray Science Division, Argonne National Laboratory, 9700 Cass Avenue, Lemont, Illinois 60439, United States

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.

View Accepted Manuscript (DOE)

Research Organization:: Argonne National Lab. (ANL), Argonne, IL (United States); Energy Frontier Research Centers (EFRC) (United States). Center for Bio-Inspired Energy Science (CBES)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)

Grant/Contract Number:: AC02-06CH11357

OSTI ID:: 1415591

Journal Information:: Journal of the American Chemical Society, Journal Name: Journal of the American Chemical Society Journal Issue: 46 Vol. 139; ISSN 0002-7863

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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DNA-Programmed Chemical Synthesis of Polymers and Inorganic Nanomaterials Xu, Xuemei; Winterwerber, Pia; Ng, David Topics in Current Chemistry, Vol. 378, Issue 2 https://doi.org/10.1007/s41061-020-0292-x	journal	March 2020
Non-equilibrium anisotropic colloidal single crystal growth with DNA Seo, Soyoung E.; Girard, Martin; Olvera de la Cruz, Monica Nature Communications, Vol. 9, Issue 1 https://doi.org/10.1038/s41467-018-06982-9	journal	November 2018
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In Situ Atomic Force Microscopy of the Reconfiguration of On‐Surface Self‐Assembled DNA‐Nanoparticle Superlattices Shekhirev, Mikhail; Sutter, Eli; Sutter, Peter Advanced Functional Materials, Vol. 29, Issue 10 https://doi.org/10.1002/adfm.201806924	journal	March 2019
Programmable Atom Equivalents: Atomic Crystallization as a Framework for Synthesizing Nanoparticle Superlattices Gabrys, Paul A.; Zornberg, Leonardo Z.; Macfarlane, Robert J. Small, Vol. 15, Issue 26 https://doi.org/10.1002/smll.201805424	journal	February 2019
Crystal engineering with DNA Laramy, Christine R.; O’Brien, Matthew N.; Mirkin, Chad A. Nature Reviews Materials, Vol. 4, Issue 3 https://doi.org/10.1038/s41578-019-0087-2	journal	February 2019

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