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Title: Molecular reorganization in bulk bottlebrush polymers: direct observation via nanoscale imaging

Abstract

Bottlebrush polymers are important for a variety of applications ranging from drug delivery to electronics. The functional flexibility of the branched sidechains has unique assembly properties when compared to linear block polymer systems. However, reports of direct observation of molecular reorganization have been sparse. This information is necessary to enhance the understanding of the structure–property relationships in these systems and yield a rational design approach for novel polymeric materials. In this work, we report direct visualization of bottlebrush molecular organization and the formation of nematic-type ordering in an amorphous polymer bottlebrush system, captured with plasma etching and helium ion microscopy. By observing the unperturbed structure of this material at high resolution and quantifying image features, we were able to qualitatively link experimental results with structures predicted by coarse-grained molecular dynamics simulations. Here, the direct visualization and computation workflow developed in this work can be applied to a broad variety of polymers with different architectures, linking imaging results with other, independent channels of information for better understanding and control of these classes of materials.

Authors:
ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [1];  [2]; ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [1]
  1. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
  2. Kimberly-Clark Corp., Irving, TX (United States)
Publication Date:
Research Org.:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Oak Ridge Leadership Computing Facility (OLCF)
Sponsoring Org.:
USDOE Office of Science (SC)
OSTI Identifier:
1515697
Grant/Contract Number:  
[AC05-00OR22725]
Resource Type:
Accepted Manuscript
Journal Name:
Nanoscale
Additional Journal Information:
[ Journal Volume: 10; Journal Issue: 37]; Journal ID: ISSN 2040-3364
Publisher:
Royal Society of Chemistry
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; Bottle brush polymers; Helium Ion Microscopy; Coarse-grained Molecular Dynamics Simulations; Image Processing

Citation Formats

Borodinov, Nikolay, Belianinov, Alex, Chang, Dongsook, Carrillo, Jan -Michael, Burch, Matthew J., Xu, Yuewen, Hong, Kunlun, Ievlev, Anton V., Sumpter, Bobby G., and Ovchinnikova, Olga S. Molecular reorganization in bulk bottlebrush polymers: direct observation via nanoscale imaging. United States: N. p., 2018. Web. doi:10.1039/C8NR05630G.
Borodinov, Nikolay, Belianinov, Alex, Chang, Dongsook, Carrillo, Jan -Michael, Burch, Matthew J., Xu, Yuewen, Hong, Kunlun, Ievlev, Anton V., Sumpter, Bobby G., & Ovchinnikova, Olga S. Molecular reorganization in bulk bottlebrush polymers: direct observation via nanoscale imaging. United States. doi:10.1039/C8NR05630G.
Borodinov, Nikolay, Belianinov, Alex, Chang, Dongsook, Carrillo, Jan -Michael, Burch, Matthew J., Xu, Yuewen, Hong, Kunlun, Ievlev, Anton V., Sumpter, Bobby G., and Ovchinnikova, Olga S. Fri . "Molecular reorganization in bulk bottlebrush polymers: direct observation via nanoscale imaging". United States. doi:10.1039/C8NR05630G. https://www.osti.gov/servlets/purl/1515697.
@article{osti_1515697,
title = {Molecular reorganization in bulk bottlebrush polymers: direct observation via nanoscale imaging},
author = {Borodinov, Nikolay and Belianinov, Alex and Chang, Dongsook and Carrillo, Jan -Michael and Burch, Matthew J. and Xu, Yuewen and Hong, Kunlun and Ievlev, Anton V. and Sumpter, Bobby G. and Ovchinnikova, Olga S.},
abstractNote = {Bottlebrush polymers are important for a variety of applications ranging from drug delivery to electronics. The functional flexibility of the branched sidechains has unique assembly properties when compared to linear block polymer systems. However, reports of direct observation of molecular reorganization have been sparse. This information is necessary to enhance the understanding of the structure–property relationships in these systems and yield a rational design approach for novel polymeric materials. In this work, we report direct visualization of bottlebrush molecular organization and the formation of nematic-type ordering in an amorphous polymer bottlebrush system, captured with plasma etching and helium ion microscopy. By observing the unperturbed structure of this material at high resolution and quantifying image features, we were able to qualitatively link experimental results with structures predicted by coarse-grained molecular dynamics simulations. Here, the direct visualization and computation workflow developed in this work can be applied to a broad variety of polymers with different architectures, linking imaging results with other, independent channels of information for better understanding and control of these classes of materials.},
doi = {10.1039/C8NR05630G},
journal = {Nanoscale},
number = [37],
volume = [10],
place = {United States},
year = {2018},
month = {9}
}

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