Side Chain Dynamics of Poly(norbornene)-g-Poly(propylene oxide) Bottlebrush Polymers

Karin J. Bichler; Bruno Jakobi; Alice Klapproth; Taiki Tominaga; Richard A. Mole; Gerald J. Schneider

doi:10.1002/marc.202200902

Side Chain Dynamics of Poly(norbornene)-g-Poly(propylene oxide) Bottlebrush Polymers

Karin J. Bichler
, Bruno Jakobi
, Alice Klapproth
, Taiki Tominaga
, Richard A. Mole
, Gerald J. Schneider

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

4 Scopus citations

Abstract

The segmental dynamics of the side chains of poly(norbornene)-g-poly(propylene oxide) (PNB-g-PPO) bottlebrush polymer in comparison to PPO is studied by quasi-elastic neutron scattering. Having experimental time and length scale information simultaneously allows to extract spatial information in addition to relaxation time. Tethering one end of the PPO side chain onto a stiff PNB backbone slows down the segmental relaxation, over the length and time scales investigated. The power law dependence of the relaxation time on the momentum transfer, Q, indicates a more heterogeneous relaxation pattern for the bottlebrush polymer, whereas the linear PPO has less deviations from a homogenous relaxation. Similar conclusions can be drawn from the time dependent mean square displacement, 〈r²(t)〉, and the non-Gaussian parameter, α₂(t). Herein, the bottlebrush polymer shows a more restricted dynamics, whereas the linear PPO reaches 〈r²(t)〉∝t^0.5at the highest temperature. The deviations from Gaussian behavior are evident at the α₂(t). Both samples show a decaying α₂(t). The non-Gaussian parameter supports the results from the power law dependence of the relaxation times, with lower α₂(t) values for PPO compared to those for PNB-g-PPO, pointing to less deviations from Gaussian behavior.

Original language	English
Article number	2200902
Journal	Macromolecular Rapid Communications
Volume	44
Issue number	7
DOIs	https://doi.org/10.1002/marc.202200902
State	Published - Apr 2023
Externally published	Yes

Funding

The authors acknowledge funding by the U.S. Department of Energy (DoE) under grant DE‐SC0019050. The authors are also grateful for the access to the neutron scattering instruments, provided by ACNS, Sydney, Australia (Pelican: P9275 and EMU: P9729) and the Materials and Life Science Experimental Facility of J‐PARC (DNA: 2022A0077). Mass spectrometry experiments were performed at the LSU Mass Spectrometry Facility (MSF). The Bruker UltrafleXtreme MALDI instrument was supported by NIH (Grant 1S10RR024520‐01A1). The authors acknowledge funding by the U.S. Department of Energy (DoE) under grant DE-SC0019050. The authors are also grateful for the access to the neutron scattering instruments, provided by ACNS, Sydney, Australia (Pelican: P9275 and EMU: P9729) and the Materials and Life Science Experimental Facility of J-PARC (DNA: 2022A0077). Mass spectrometry experiments were performed at the LSU Mass Spectrometry Facility (MSF). The Bruker UltrafleXtreme MALDI instrument was supported by NIH (Grant 1S10RR024520-01A1).

Keywords

bottlebrush polymers
neutron scattering
segmental dynamics

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10.1002/marc.202200902

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title = "Side Chain Dynamics of Poly(norbornene)-g-Poly(propylene oxide) Bottlebrush Polymers",

abstract = "The segmental dynamics of the side chains of poly(norbornene)-g-poly(propylene oxide) (PNB-g-PPO) bottlebrush polymer in comparison to PPO is studied by quasi-elastic neutron scattering. Having experimental time and length scale information simultaneously allows to extract spatial information in addition to relaxation time. Tethering one end of the PPO side chain onto a stiff PNB backbone slows down the segmental relaxation, over the length and time scales investigated. The power law dependence of the relaxation time on the momentum transfer, Q, indicates a more heterogeneous relaxation pattern for the bottlebrush polymer, whereas the linear PPO has less deviations from a homogenous relaxation. Similar conclusions can be drawn from the time dependent mean square displacement, 〈r2(t)〉, and the non-Gaussian parameter, α2(t). Herein, the bottlebrush polymer shows a more restricted dynamics, whereas the linear PPO reaches 〈r2(t)〉∝t0.5at the highest temperature. The deviations from Gaussian behavior are evident at the α2(t). Both samples show a decaying α2(t). The non-Gaussian parameter supports the results from the power law dependence of the relaxation times, with lower α2(t) values for PPO compared to those for PNB-g-PPO, pointing to less deviations from Gaussian behavior.",

keywords = "bottlebrush polymers, neutron scattering, segmental dynamics",

author = "Bichler, \{Karin J.\} and Bruno Jakobi and Alice Klapproth and Taiki Tominaga and Mole, \{Richard A.\} and Schneider, \{Gerald J.\}",

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AU - Bichler, Karin J.

AU - Jakobi, Bruno

AU - Klapproth, Alice

AU - Tominaga, Taiki

AU - Mole, Richard A.

AU - Schneider, Gerald J.

PY - 2023/4

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N2 - The segmental dynamics of the side chains of poly(norbornene)-g-poly(propylene oxide) (PNB-g-PPO) bottlebrush polymer in comparison to PPO is studied by quasi-elastic neutron scattering. Having experimental time and length scale information simultaneously allows to extract spatial information in addition to relaxation time. Tethering one end of the PPO side chain onto a stiff PNB backbone slows down the segmental relaxation, over the length and time scales investigated. The power law dependence of the relaxation time on the momentum transfer, Q, indicates a more heterogeneous relaxation pattern for the bottlebrush polymer, whereas the linear PPO has less deviations from a homogenous relaxation. Similar conclusions can be drawn from the time dependent mean square displacement, 〈r2(t)〉, and the non-Gaussian parameter, α2(t). Herein, the bottlebrush polymer shows a more restricted dynamics, whereas the linear PPO reaches 〈r2(t)〉∝t0.5at the highest temperature. The deviations from Gaussian behavior are evident at the α2(t). Both samples show a decaying α2(t). The non-Gaussian parameter supports the results from the power law dependence of the relaxation times, with lower α2(t) values for PPO compared to those for PNB-g-PPO, pointing to less deviations from Gaussian behavior.

AB - The segmental dynamics of the side chains of poly(norbornene)-g-poly(propylene oxide) (PNB-g-PPO) bottlebrush polymer in comparison to PPO is studied by quasi-elastic neutron scattering. Having experimental time and length scale information simultaneously allows to extract spatial information in addition to relaxation time. Tethering one end of the PPO side chain onto a stiff PNB backbone slows down the segmental relaxation, over the length and time scales investigated. The power law dependence of the relaxation time on the momentum transfer, Q, indicates a more heterogeneous relaxation pattern for the bottlebrush polymer, whereas the linear PPO has less deviations from a homogenous relaxation. Similar conclusions can be drawn from the time dependent mean square displacement, 〈r2(t)〉, and the non-Gaussian parameter, α2(t). Herein, the bottlebrush polymer shows a more restricted dynamics, whereas the linear PPO reaches 〈r2(t)〉∝t0.5at the highest temperature. The deviations from Gaussian behavior are evident at the α2(t). Both samples show a decaying α2(t). The non-Gaussian parameter supports the results from the power law dependence of the relaxation times, with lower α2(t) values for PPO compared to those for PNB-g-PPO, pointing to less deviations from Gaussian behavior.

KW - bottlebrush polymers

KW - neutron scattering

KW - segmental dynamics

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Side Chain Dynamics of Poly(norbornene)-g-Poly(propylene oxide) Bottlebrush Polymers

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