Dynamics of Bottlebrush Polymers in Solution by Neutron Spin Echo Spectroscopy

Karin J. Bichler; Bruno Jakobi; Dirk Honecker; Laura R. Stingaciu; Thomas K. Weldeghiorghis; James H.P. Collins; Gerald J. Schneider

doi:10.1021/acs.macromol.2c01177

Dynamics of Bottlebrush Polymers in Solution by Neutron Spin Echo Spectroscopy

Karin J. Bichler, Bruno Jakobi, Dirk Honecker, Laura R. Stingaciu, Thomas K. Weldeghiorghis, James H.P. Collins, Gerald J. Schneider

SANS & Spin Echo

Research output: Contribution to journal › Article › peer-review

3 Scopus citations

Abstract

We present dynamical and morphological studies on poly(dimethylsiloxane) (PDMS)-based bottlebrush polymers in solution. A combination of small-angle neutron scattering (SANS), pulsed field gradient nuclear magnetic resonance (PFG NMR), and neutron spin echo (NSE) spectroscopy was used to identify structural changes inherent in changing the side-chain length while keeping the backbone constant. These morphological changes are mirrored in the diffusion coefficient determined by PFG NMR, resulting in two coefficients for the elongated and one for the more spherical sample. Faster motions are tracked by NSE using the advantage of time- and length-scale resolutions with the diffusion coefficient predetermined by PFG NMR. Hereby, the sample with short side chains relaxes like wormlike micelles considering the longitudinal direction, whereas the dynamics along the radial extension shows a much stronger Q-dependence as known from any theory. The dynamical behavior within the blob region, covered with the more spherical sample, follows the predictions of Zimm as well as of Zilman and Granek (ZG).

Original language	English
Pages (from-to)	9810-9819
Number of pages	10
Journal	Macromolecules
Volume	55
Issue number	21
DOIs	https://doi.org/10.1021/acs.macromol.2c01177
State	Published - Nov 8 2022

Funding

The authors acknowledge funding by the U.S. Department of Energy under Grant number DE-SC0019050. This research used resources at the Spallation Neutron Source, a DOE Office of Science User Facility operated by the Oak Ridge National Laboratory. Experiments at the ISIS Pulsed Neutron and Muon Source were supported by a beamtime allocation from the Science and Technology Facilities’ Council (10.5286/ISIS.E.RB1920275). A portion of this work was performed in the McKnight Brain Institute at the National High Magnetic Field Laboratory’s Advanced Magnetic Resonance Imaging and Spectroscopy (AMRIS) Facility, which was supported by National Science Foundation Cooperative Agreement No. DMR-1644779 and the State of Florida.

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title = "Dynamics of Bottlebrush Polymers in Solution by Neutron Spin Echo Spectroscopy",

abstract = "We present dynamical and morphological studies on poly(dimethylsiloxane) (PDMS)-based bottlebrush polymers in solution. A combination of small-angle neutron scattering (SANS), pulsed field gradient nuclear magnetic resonance (PFG NMR), and neutron spin echo (NSE) spectroscopy was used to identify structural changes inherent in changing the side-chain length while keeping the backbone constant. These morphological changes are mirrored in the diffusion coefficient determined by PFG NMR, resulting in two coefficients for the elongated and one for the more spherical sample. Faster motions are tracked by NSE using the advantage of time- and length-scale resolutions with the diffusion coefficient predetermined by PFG NMR. Hereby, the sample with short side chains relaxes like wormlike micelles considering the longitudinal direction, whereas the dynamics along the radial extension shows a much stronger Q-dependence as known from any theory. The dynamical behavior within the blob region, covered with the more spherical sample, follows the predictions of Zimm as well as of Zilman and Granek (ZG).",

author = "Bichler, {Karin J.} and Bruno Jakobi and Dirk Honecker and Stingaciu, {Laura R.} and Weldeghiorghis, {Thomas K.} and Collins, {James H.P.} and Schneider, {Gerald J.}",

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AU - Bichler, Karin J.

AU - Jakobi, Bruno

AU - Honecker, Dirk

AU - Stingaciu, Laura R.

AU - Weldeghiorghis, Thomas K.

AU - Collins, James H.P.

AU - Schneider, Gerald J.

PY - 2022/11/8

Y1 - 2022/11/8

N2 - We present dynamical and morphological studies on poly(dimethylsiloxane) (PDMS)-based bottlebrush polymers in solution. A combination of small-angle neutron scattering (SANS), pulsed field gradient nuclear magnetic resonance (PFG NMR), and neutron spin echo (NSE) spectroscopy was used to identify structural changes inherent in changing the side-chain length while keeping the backbone constant. These morphological changes are mirrored in the diffusion coefficient determined by PFG NMR, resulting in two coefficients for the elongated and one for the more spherical sample. Faster motions are tracked by NSE using the advantage of time- and length-scale resolutions with the diffusion coefficient predetermined by PFG NMR. Hereby, the sample with short side chains relaxes like wormlike micelles considering the longitudinal direction, whereas the dynamics along the radial extension shows a much stronger Q-dependence as known from any theory. The dynamical behavior within the blob region, covered with the more spherical sample, follows the predictions of Zimm as well as of Zilman and Granek (ZG).

AB - We present dynamical and morphological studies on poly(dimethylsiloxane) (PDMS)-based bottlebrush polymers in solution. A combination of small-angle neutron scattering (SANS), pulsed field gradient nuclear magnetic resonance (PFG NMR), and neutron spin echo (NSE) spectroscopy was used to identify structural changes inherent in changing the side-chain length while keeping the backbone constant. These morphological changes are mirrored in the diffusion coefficient determined by PFG NMR, resulting in two coefficients for the elongated and one for the more spherical sample. Faster motions are tracked by NSE using the advantage of time- and length-scale resolutions with the diffusion coefficient predetermined by PFG NMR. Hereby, the sample with short side chains relaxes like wormlike micelles considering the longitudinal direction, whereas the dynamics along the radial extension shows a much stronger Q-dependence as known from any theory. The dynamical behavior within the blob region, covered with the more spherical sample, follows the predictions of Zimm as well as of Zilman and Granek (ZG).

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Dynamics of Bottlebrush Polymers in Solution by Neutron Spin Echo Spectroscopy

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