Influence of Liquid Crystallinity and Mechanical Deformation on the Molecular Relaxations of an Auxetic Liquid Crystal Elastomer

Liquid Crystal Elastomers (LCEs) combine the anisotropic ordering of liquid crystals with the elastic properties of elastomers, providing unique physical properties, such as stimuli responsiveness and a recently discovered molecular auxetic response. Here, we determine how the molecular relaxation d...

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Published inMolecules (Basel, Switzerland) Vol. 26; no. 23; p. 7313
Main Authors Raistrick, Thomas, Reynolds, Matthew, Gleeson, Helen F, Mattsson, Johan
Format Journal Article
LanguageEnglish
Published Switzerland MDPI AG 02.12.2021
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Abstract Liquid Crystal Elastomers (LCEs) combine the anisotropic ordering of liquid crystals with the elastic properties of elastomers, providing unique physical properties, such as stimuli responsiveness and a recently discovered molecular auxetic response. Here, we determine how the molecular relaxation dynamics in an acrylate LCE are affected by its phase using broadband dielectric relaxation spectroscopy, calorimetry and rheology. Our LCE is an excellent model system since it exhibits a molecular auxetic response in its nematic state, and chemically identical nematic or isotropic samples can be prepared by cross-linking. We find that the glass transition temperatures (Tg) and dynamic fragilities are similar in both phases, and the T-dependence of the α relaxation shows a crossover at the same T* for both phases. However, for T>T*, the behavior becomes Arrhenius for the nematic LCE, but only more Arrhenius-like for the isotropic sample. We provide evidence that the latter behavior is related to the existence of pre-transitional nematic fluctuations in the isotropic LCE, which are locked in by polymerization. The role of applied strain on the relaxation dynamics and mechanical response of the LCE is investigated; this is particularly important since the molecular auxetic response is linked to a mechanical Fréedericksz transition that is not fully understood. We demonstrate that the complex Young's modulus and the α relaxation time remain relatively unchanged for small deformations, whereas for strains for which the auxetic response is achieved, significant increases are observed. We suggest that the observed molecular auxetic response is coupled to the strain-induced out-of-plane rotation of the mesogen units, in turn driven by the increasing constraints on polymer configurations, as reflected in increasing elastic moduli and α relaxation times; this is consistent with our recent results showing that the auxetic response coincides with the emergence of biaxial order.
AbstractList Liquid Crystal Elastomers (LCEs) combine the anisotropic ordering of liquid crystals with the elastic properties of elastomers, providing unique physical properties, such as stimuli responsiveness and a recently discovered molecular auxetic response. Here, we determine how the molecular relaxation dynamics in an acrylate LCE are affected by its phase using broadband dielectric relaxation spectroscopy, calorimetry and rheology. Our LCE is an excellent model system since it exhibits a molecular auxetic response in its nematic state, and chemically identical nematic or isotropic samples can be prepared by cross-linking. We find that the glass transition temperatures (Tg) and dynamic fragilities are similar in both phases, and the T-dependence of the α relaxation shows a crossover at the same T* for both phases. However, for T>T*, the behavior becomes Arrhenius for the nematic LCE, but only more Arrhenius-like for the isotropic sample. We provide evidence that the latter behavior is related to the existence of pre-transitional nematic fluctuations in the isotropic LCE, which are locked in by polymerization. The role of applied strain on the relaxation dynamics and mechanical response of the LCE is investigated; this is particularly important since the molecular auxetic response is linked to a mechanical Fréedericksz transition that is not fully understood. We demonstrate that the complex Young's modulus and the α relaxation time remain relatively unchanged for small deformations, whereas for strains for which the auxetic response is achieved, significant increases are observed. We suggest that the observed molecular auxetic response is coupled to the strain-induced out-of-plane rotation of the mesogen units, in turn driven by the increasing constraints on polymer configurations, as reflected in increasing elastic moduli and α relaxation times; this is consistent with our recent results showing that the auxetic response coincides with the emergence of biaxial order.
Liquid Crystal Elastomers (LCEs) combine the anisotropic ordering of liquid crystals with the elastic properties of elastomers, providing unique physical properties, such as stimuli responsiveness and a recently discovered molecular auxetic response. Here, we determine how the molecular relaxation dynamics in an acrylate LCE are affected by its phase using broadband dielectric relaxation spectroscopy, calorimetry and rheology. Our LCE is an excellent model system since it exhibits a molecular auxetic response in its nematic state, and chemically identical nematic or isotropic samples can be prepared by cross-linking. We find that the glass transition temperatures ( T g ) and dynamic fragilities are similar in both phases, and the T -dependence of the α relaxation shows a crossover at the same T* for both phases. However, for T>T* , the behavior becomes Arrhenius for the nematic LCE, but only more Arrhenius-like for the isotropic sample. We provide evidence that the latter behavior is related to the existence of pre-transitional nematic fluctuations in the isotropic LCE, which are locked in by polymerization. The role of applied strain on the relaxation dynamics and mechanical response of the LCE is investigated; this is particularly important since the molecular auxetic response is linked to a mechanical Fréedericksz transition that is not fully understood. We demonstrate that the complex Young’s modulus and the α relaxation time remain relatively unchanged for small deformations, whereas for strains for which the auxetic response is achieved, significant increases are observed. We suggest that the observed molecular auxetic response is coupled to the strain-induced out-of-plane rotation of the mesogen units, in turn driven by the increasing constraints on polymer configurations, as reflected in increasing elastic moduli and α relaxation times; this is consistent with our recent results showing that the auxetic response coincides with the emergence of biaxial order.
Liquid Crystal Elastomers (LCEs) combine the anisotropic ordering of liquid crystals with the elastic properties of elastomers, providing unique physical properties, such as stimuli responsiveness and a recently discovered molecular auxetic response. Here, we determine how the molecular relaxation dynamics in an acrylate LCE are affected by its phase using broadband dielectric relaxation spectroscopy, calorimetry and rheology. Our LCE is an excellent model system since it exhibits a molecular auxetic response in its nematic state, and chemically identical nematic or isotropic samples can be prepared by cross-linking. We find that the glass transition temperatures ( T g ) and dynamic fragilities are similar in both phases, and the T -dependence of the α relaxation shows a crossover at the same T * for both phases. However, for T > T * , the behavior becomes Arrhenius for the nematic LCE, but only more Arrhenius-like for the isotropic sample. We provide evidence that the latter behavior is related to the existence of pre-transitional nematic fluctuations in the isotropic LCE, which are locked in by polymerization. The role of applied strain on the relaxation dynamics and mechanical response of the LCE is investigated; this is particularly important since the molecular auxetic response is linked to a mechanical Fréedericksz transition that is not fully understood. We demonstrate that the complex Young’s modulus and the α relaxation time remain relatively unchanged for small deformations, whereas for strains for which the auxetic response is achieved, significant increases are observed. We suggest that the observed molecular auxetic response is coupled to the strain-induced out-of-plane rotation of the mesogen units, in turn driven by the increasing constraints on polymer configurations, as reflected in increasing elastic moduli and α relaxation times; this is consistent with our recent results showing that the auxetic response coincides with the emergence of biaxial order.
Author Mattsson, Johan
Reynolds, Matthew
Gleeson, Helen F
Raistrick, Thomas
AuthorAffiliation School of Physics and Astronomy, University of Leeds, Leeds LS2 9JT, UK; py14tr@leeds.ac.uk (T.R.); M.Reynolds@leeds.ac.uk (M.R.); h.f.gleeson@leeds.ac.uk (H.F.G.)
AuthorAffiliation_xml – name: School of Physics and Astronomy, University of Leeds, Leeds LS2 9JT, UK; py14tr@leeds.ac.uk (T.R.); M.Reynolds@leeds.ac.uk (M.R.); h.f.gleeson@leeds.ac.uk (H.F.G.)
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  givenname: Thomas
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  surname: Raistrick
  fullname: Raistrick, Thomas
  organization: School of Physics and Astronomy, University of Leeds, Leeds LS2 9JT, UK
– sequence: 2
  givenname: Matthew
  surname: Reynolds
  fullname: Reynolds, Matthew
  organization: School of Physics and Astronomy, University of Leeds, Leeds LS2 9JT, UK
– sequence: 3
  givenname: Helen F
  orcidid: 0000-0002-7494-2100
  surname: Gleeson
  fullname: Gleeson, Helen F
  organization: School of Physics and Astronomy, University of Leeds, Leeds LS2 9JT, UK
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  givenname: Johan
  surname: Mattsson
  fullname: Mattsson, Johan
  organization: School of Physics and Astronomy, University of Leeds, Leeds LS2 9JT, UK
BackLink https://www.ncbi.nlm.nih.gov/pubmed/34885896$$D View this record in MEDLINE/PubMed
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Issue 23
Keywords liquid crystalline elastomer
dielectric spectroscopy
polymer relaxations
shear rheology
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Snippet Liquid Crystal Elastomers (LCEs) combine the anisotropic ordering of liquid crystals with the elastic properties of elastomers, providing unique physical...
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StartPage 7313
SubjectTerms Behavior
Broadband
Calorimetry
Cooling
Crosslinking
Crystals
Deformation
Dielectric relaxation
dielectric spectroscopy
Elastic anisotropy
Elastic properties
Elastomers
Energy
Freedericksz transitions
Glass
Glass transition temperature
liquid crystalline elastomer
Liquid crystals
Mechanical properties
Modulus of elasticity
Molecular relaxation
Phase transitions
Physical properties
Polymer melts
polymer relaxations
Polymers
Relaxation time
Rheological properties
Rheology
shear rheology
Spectroscopy
Strain
Transition temperatures
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Title Influence of Liquid Crystallinity and Mechanical Deformation on the Molecular Relaxations of an Auxetic Liquid Crystal Elastomer
URI https://www.ncbi.nlm.nih.gov/pubmed/34885896
https://www.proquest.com/docview/2608136933
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https://pubmed.ncbi.nlm.nih.gov/PMC8659252
https://doaj.org/article/fdc74deb00dd4229bfe29ed1981b0088
Volume 26
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