Universality of Time-Temperature Scaling Observed by Neutron Spectroscopy on Bottlebrush Polymers

Karin J. Bichler; Bruno Jakobi; Victoria García Sakai; Alice Klapproth; Richard A. Mole; Gerald J. Schneider

doi:10.1021/acs.nanolett.1c01379

Universality of Time-Temperature Scaling Observed by Neutron Spectroscopy on Bottlebrush Polymers

Karin J. Bichler
, Bruno Jakobi
, Victoria García Sakai
, Alice Klapproth
, Richard A. Mole
, Gerald J. Schneider

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

8 Scopus citations

Abstract

The understanding of materials requires access to the dynamics over many orders of magnitude in time; however, single analytical techniques are restricted in their respective time ranges. Assuming a functional relationship between time and temperature is one viable tool to overcome these limits. Despite its frequent usage, a breakdown of this assertion at the glass-transition temperature is common. Here, we take advantage of time- and length-scale information in neutron spectroscopy to show that the separation of different processes is the minimum requirement toward a more universal picture at, and even below, the glass transition for our systems. This is illustrated by constructing the full proton mean-square displacement for three bottlebrush polymers from femto- to nanoseconds, with simultaneous information on the partial contributions from segmental relaxation, methyl group rotation, and vibrations. The information can be used for a better analysis of results from numerous techniques and samples, improving the overall understanding of materials properties.

Original language	English
Pages (from-to)	4494-4499
Number of pages	6
Journal	Nano Letters
Volume	21
Issue number	10
DOIs	https://doi.org/10.1021/acs.nanolett.1c01379
State	Published - May 26 2021
Externally published	Yes

Funding

We gratefully acknowledge funding by the U.S. Department of Energy (DoE) under grant DE-SC0019050. We also would like to acknowledge ACNS (P7387 and P7389), Sydney, Australia, and the ISIS Neutron and Muon Facility (DOI: 10.5286/ISIS.E.RB1910220), Didcot, United Kingdom, for access to the quasi-elastic neutron scattering instruments. We thank Prof. David Spivak (Department of Chemistry, Louisiana State University) for carefully proofreading the manuscript.

Keywords

Bottlebrush Polymer
Polydimethylsiloxane
Quasi-Elastic Neutron Scattering
Time-Temperature Superposition

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10.1021/acs.nanolett.1c01379

Cite this

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title = "Universality of Time-Temperature Scaling Observed by Neutron Spectroscopy on Bottlebrush Polymers",

abstract = "The understanding of materials requires access to the dynamics over many orders of magnitude in time; however, single analytical techniques are restricted in their respective time ranges. Assuming a functional relationship between time and temperature is one viable tool to overcome these limits. Despite its frequent usage, a breakdown of this assertion at the glass-transition temperature is common. Here, we take advantage of time- and length-scale information in neutron spectroscopy to show that the separation of different processes is the minimum requirement toward a more universal picture at, and even below, the glass transition for our systems. This is illustrated by constructing the full proton mean-square displacement for three bottlebrush polymers from femto- to nanoseconds, with simultaneous information on the partial contributions from segmental relaxation, methyl group rotation, and vibrations. The information can be used for a better analysis of results from numerous techniques and samples, improving the overall understanding of materials properties.",

keywords = "Bottlebrush Polymer, Polydimethylsiloxane, Quasi-Elastic Neutron Scattering, Time-Temperature Superposition",

author = "Bichler, \{Karin J.\} and Bruno Jakobi and Sakai, \{Victoria Garc{\'i}a\} and Alice Klapproth and Mole, \{Richard A.\} and Schneider, \{Gerald J.\}",

note = "Publisher Copyright: {\textcopyright} 2021 The Authors. Published by American Chemical Society.",

year = "2021",

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doi = "10.1021/acs.nanolett.1c01379",

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T1 - Universality of Time-Temperature Scaling Observed by Neutron Spectroscopy on Bottlebrush Polymers

AU - Bichler, Karin J.

AU - Jakobi, Bruno

AU - Sakai, Victoria García

AU - Klapproth, Alice

AU - Mole, Richard A.

AU - Schneider, Gerald J.

PY - 2021/5/26

Y1 - 2021/5/26

N2 - The understanding of materials requires access to the dynamics over many orders of magnitude in time; however, single analytical techniques are restricted in their respective time ranges. Assuming a functional relationship between time and temperature is one viable tool to overcome these limits. Despite its frequent usage, a breakdown of this assertion at the glass-transition temperature is common. Here, we take advantage of time- and length-scale information in neutron spectroscopy to show that the separation of different processes is the minimum requirement toward a more universal picture at, and even below, the glass transition for our systems. This is illustrated by constructing the full proton mean-square displacement for three bottlebrush polymers from femto- to nanoseconds, with simultaneous information on the partial contributions from segmental relaxation, methyl group rotation, and vibrations. The information can be used for a better analysis of results from numerous techniques and samples, improving the overall understanding of materials properties.

AB - The understanding of materials requires access to the dynamics over many orders of magnitude in time; however, single analytical techniques are restricted in their respective time ranges. Assuming a functional relationship between time and temperature is one viable tool to overcome these limits. Despite its frequent usage, a breakdown of this assertion at the glass-transition temperature is common. Here, we take advantage of time- and length-scale information in neutron spectroscopy to show that the separation of different processes is the minimum requirement toward a more universal picture at, and even below, the glass transition for our systems. This is illustrated by constructing the full proton mean-square displacement for three bottlebrush polymers from femto- to nanoseconds, with simultaneous information on the partial contributions from segmental relaxation, methyl group rotation, and vibrations. The information can be used for a better analysis of results from numerous techniques and samples, improving the overall understanding of materials properties.

KW - Bottlebrush Polymer

KW - Polydimethylsiloxane

KW - Quasi-Elastic Neutron Scattering

KW - Time-Temperature Superposition

UR - https://www.scopus.com/pages/publications/85106481408

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SN - 1530-6984

VL - 21

SP - 4494

EP - 4499

JO - Nano Letters

JF - Nano Letters

IS - 10

ER -

Universality of Time-Temperature Scaling Observed by Neutron Spectroscopy on Bottlebrush Polymers

Abstract

Funding

Keywords

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