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Title: Divalent Multilinking Bonds Control Growth and Morphology of Nanopolymers

Abstract

Assembly of nanoscale objects into linear architectures resembling molecular polymers is a basic organization resulting from divalent interactions. Such linear architectures occur for particles with two binding patches on opposite sides, known as Janus particles. However, unlike molecular systems where valence bonds can be envisioned as pointlike interactions nanoscale patches are often realized through multiple molecular linkages. The relationship between the characteristics of these linkages, the resulting interpatch connectivity, and assembly morphology is not well-explored. Here, we investigate assembly behavior of model divalent nanomonomers, DNA nanocuboid with tailorable multilinking bonds. Our study reveals that the characteristics of individual molecular linkages and their collective properties have a profound effect on nanomonomer reactivity and resulting morphologies. Beyond linear nanopolymers, a common signature of divalent nanomonomers, we observe an effective valence increase as linkages lengthened, leading to the nanopolymer bundling. The experimental findings are rationalized by molecular dynamics simulations.

Authors:
ORCiD logo [1]; ORCiD logo [1];  [2];  [1];  [3];  [1];  [4];  [5]; ORCiD logo [6]; ORCiD logo [7]
  1. Department of Chemical Engineering, Columbia University, New York, New York 10027, United States
  2. Computational and Soft Matter Physics, Faculty of Physics, University of Vienna, Boltzmanngasse 5, 1090 Vienna, Austria, MMM Mathematics-Magnetism-Materials, Research Platform, University of Vienna, Boltzmanngasse 5, 1090 Vienna, Austria
  3. Department of Applied Physics and Applied Mathematics, Columbia University, New York, New York 10027, United States
  4. Computational and Soft Matter Physics, Faculty of Physics, University of Vienna, Boltzmanngasse 5, 1090 Vienna, Austria
  5. Computational and Soft Matter Physics, Faculty of Physics, University of Vienna, Boltzmanngasse 5, 1090 Vienna, Austria, Department of Mathematical and Theoretical Physics, Institute of Mathematics and Natural Sciences, Ural Federal University, Ekaterinburg, 620026, Russia, MMM Mathematics-Magnetism-Materials, Research Platform, University of Vienna, Boltzmanngasse 5, 1090 Vienna, Austria
  6. Wallace H. Coulter Department of Biomedical Engineering, Georgia Institute of Technology and Emory University, Atlanta, Georgia 30322, United States
  7. Department of Chemical Engineering, Columbia University, New York, New York 10027, United States, Department of Applied Physics and Applied Mathematics, Columbia University, New York, New York 10027, United States, Center for Functional Nanomaterials, Brookhaven National Laboratory, Upton, New York 11973, United States
Publication Date:
Research Org.:
Columbia Univ., New York, NY (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1826246
Alternate Identifier(s):
OSTI ID: 1837168
Grant/Contract Number:  
SC0008772; SC0012704
Resource Type:
Published Article
Journal Name:
Nano Letters
Additional Journal Information:
Journal Name: Nano Letters Journal Volume: 21 Journal Issue: 24; Journal ID: ISSN 1530-6984
Publisher:
American Chemical Society
Country of Publication:
United States
Language:
English
Subject:
77 NANOSCIENCE AND NANOTECHNOLOGY; patchy particles; DNA nanotechnology; self-assembly; polymerization; phase behavior; polymer morphology; genetics; nanoparticles; reactivity

Citation Formats

Xiong, Yan, Lin, Zhiwei, Mostarac, Deniz, Minevich, Brian, Peng, Qiuyuan, Zhu, Guolong, Sánchez, Pedro A., Kantorovich, Sofia, Ke, Yonggang, and Gang, Oleg. Divalent Multilinking Bonds Control Growth and Morphology of Nanopolymers. United States: N. p., 2021. Web. doi:10.1021/acs.nanolett.1c03009.
Xiong, Yan, Lin, Zhiwei, Mostarac, Deniz, Minevich, Brian, Peng, Qiuyuan, Zhu, Guolong, Sánchez, Pedro A., Kantorovich, Sofia, Ke, Yonggang, & Gang, Oleg. Divalent Multilinking Bonds Control Growth and Morphology of Nanopolymers. United States. https://doi.org/10.1021/acs.nanolett.1c03009
Xiong, Yan, Lin, Zhiwei, Mostarac, Deniz, Minevich, Brian, Peng, Qiuyuan, Zhu, Guolong, Sánchez, Pedro A., Kantorovich, Sofia, Ke, Yonggang, and Gang, Oleg. Thu . "Divalent Multilinking Bonds Control Growth and Morphology of Nanopolymers". United States. https://doi.org/10.1021/acs.nanolett.1c03009.
@article{osti_1826246,
title = {Divalent Multilinking Bonds Control Growth and Morphology of Nanopolymers},
author = {Xiong, Yan and Lin, Zhiwei and Mostarac, Deniz and Minevich, Brian and Peng, Qiuyuan and Zhu, Guolong and Sánchez, Pedro A. and Kantorovich, Sofia and Ke, Yonggang and Gang, Oleg},
abstractNote = {Assembly of nanoscale objects into linear architectures resembling molecular polymers is a basic organization resulting from divalent interactions. Such linear architectures occur for particles with two binding patches on opposite sides, known as Janus particles. However, unlike molecular systems where valence bonds can be envisioned as pointlike interactions nanoscale patches are often realized through multiple molecular linkages. The relationship between the characteristics of these linkages, the resulting interpatch connectivity, and assembly morphology is not well-explored. Here, we investigate assembly behavior of model divalent nanomonomers, DNA nanocuboid with tailorable multilinking bonds. Our study reveals that the characteristics of individual molecular linkages and their collective properties have a profound effect on nanomonomer reactivity and resulting morphologies. Beyond linear nanopolymers, a common signature of divalent nanomonomers, we observe an effective valence increase as linkages lengthened, leading to the nanopolymer bundling. The experimental findings are rationalized by molecular dynamics simulations.},
doi = {10.1021/acs.nanolett.1c03009},
journal = {Nano Letters},
number = 24,
volume = 21,
place = {United States},
year = {2021},
month = {10}
}

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