On the equivalence between the thermodynamic and dynamic measurements of the glass transition in confined polymers

Understanding why the glass transition temperature (Tg) of polymers deviates substantially from the bulk with nanoscale confinement has been a 20-year mystery. Ever since the observation in the mid-1990s that the Tg values of amorphous polymer thin films are different from their bulk values, efforts...

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Published inJournal of non-crystalline solids Vol. 407; pp. 288 - 295
Main Authors Priestley, Rodney D., Cangialosi, Daniele, Napolitano, Simone
Format Journal Article
LanguageEnglish
Published Elsevier B.V 01.01.2015
Subjects
Chain adsorption
Confinement
Decoupling
Dynamic tests
Dynamics
Free volume
Glass transition
Glassy
Polymer thin films
Polymers
Thin films
Glass transition
Free volume
Polymer thin films
Chain adsorption
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Abstract Understanding why the glass transition temperature (Tg) of polymers deviates substantially from the bulk with nanoscale confinement has been a 20-year mystery. Ever since the observation in the mid-1990s that the Tg values of amorphous polymer thin films are different from their bulk values, efforts to understand this behavior have intensified, and the topic remains the subject of intense research and debate. This is due to the combined scientific and technological implications of size-dependent glassy properties. Here, we discuss an intriguing aspect of the glassy behavior of confined amorphous polymers. As experimentally assessed, the glass transition is a dynamic event mediated by segmental dynamics. Thus, it seems intuitive to expect that a change in Tg due to confinement necessitates a corresponding change in molecular dynamics, and that such change in dynamics may be predicted based on our understanding of the glass transition. The aim of this perspectives article is to examine whether or not segmental dynamics change in accordance with the value of Tg for confined polymers based on bulk rules. We highlight past and recent findings that have examined the relationship between Tg and segmental dynamics of confined polymers. Within this context, the decoupling between these two aspects of the glass transition in confinement is emphasized. We discuss these results within the framework of our current understanding of the glass transition as well as efforts to resolve this decoupling. Finally, the anomalous decoupling between translational (diffusion) and rotational (segmental) motion taking place in the proximity of attractive interfaces in polymer thin films is discussed. •The glass transition in confined polymers is reviewed.•Dynamic and pseudo-thermodynamic measurements of Tg are decoupled in confinement.•Free volume diffusion and chain adsorption offer insight into decoupling.
AbstractList Understanding why the glass transition temperature (Tg ) of polymers deviates substantially from the bulk with nanoscale confinement has been a 20-year mystery. Ever since the observation in the mid-1990s that the Tg values of amorphous polymer thin films are different from their bulk values, efforts to understand this behavior have intensified, and the topic remains the subject of intense research and debate. This is due to the combined scientific and technological implications of size-dependent glassy properties. Here, we discuss an intriguing aspect of the glassy behavior of confined amorphous polymers. As experimentally assessed, the glass transition is a dynamic event mediated by segmental dynamics. Thus, it seems intuitive to expect that a change in Tg due to confinement necessitates a corresponding change in molecular dynamics, and that such change in dynamics may be predicted based on our understanding of the glass transition. The aim of this perspectives article is to examine whether or not segmental dynamics change in accordance with the value of Tg for confined polymers based on bulk rules. We highlight past and recent findings that have examined the relationship between Tg and segmental dynamics of confined polymers. Within this context, the decoupling between these two aspects of the glass transition in confinement is emphasized. We discuss these results within the framework of our current understanding of the glass transition as well as efforts to resolve this decoupling. Finally, the anomalous decoupling between translational (diffusion) and rotational (segmental) motion taking place in the proximity of attractive interfaces in polymer thin films is discussed.
Understanding why the glass transition temperature (Tg) of polymers deviates substantially from the bulk with nanoscale confinement has been a 20-year mystery. Ever since the observation in the mid-1990s that the Tg values of amorphous polymer thin films are different from their bulk values, efforts to understand this behavior have intensified, and the topic remains the subject of intense research and debate. This is due to the combined scientific and technological implications of size-dependent glassy properties. Here, we discuss an intriguing aspect of the glassy behavior of confined amorphous polymers. As experimentally assessed, the glass transition is a dynamic event mediated by segmental dynamics. Thus, it seems intuitive to expect that a change in Tg due to confinement necessitates a corresponding change in molecular dynamics, and that such change in dynamics may be predicted based on our understanding of the glass transition. The aim of this perspectives article is to examine whether or not segmental dynamics change in accordance with the value of Tg for confined polymers based on bulk rules. We highlight past and recent findings that have examined the relationship between Tg and segmental dynamics of confined polymers. Within this context, the decoupling between these two aspects of the glass transition in confinement is emphasized. We discuss these results within the framework of our current understanding of the glass transition as well as efforts to resolve this decoupling. Finally, the anomalous decoupling between translational (diffusion) and rotational (segmental) motion taking place in the proximity of attractive interfaces in polymer thin films is discussed. •The glass transition in confined polymers is reviewed.•Dynamic and pseudo-thermodynamic measurements of Tg are decoupled in confinement.•Free volume diffusion and chain adsorption offer insight into decoupling.
Author Cangialosi, Daniele
Napolitano, Simone
Priestley, Rodney D.
Author_xml – sequence: 1
  givenname: Rodney D.
  surname: Priestley
  fullname: Priestley, Rodney D.
  email: rpriestl@princeton.edu
  organization: Department of Chemical and Biological Engineering, Princeton University, Princeton, NJ 08544, USA
– sequence: 2
  givenname: Daniele
  surname: Cangialosi
  fullname: Cangialosi, Daniele
  email: swxcacad@sc.ehu.es
  organization: Centro de Física de Materiales (CSIC-UPV/EHU), Paseo Manuel de Lardizábal 5, San Sebastián 20018, Spain
– sequence: 3
  givenname: Simone
  surname: Napolitano
  fullname: Napolitano, Simone
  email: snapolit@ulb.ac.be
  organization: Laboratory of Polymer and Soft Matter Dynamics, Faculté de Science, Université Libre de Bruxelles (ULB), Bruxelles 1050, Belgium
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Snippet Understanding why the glass transition temperature (Tg) of polymers deviates substantially from the bulk with nanoscale confinement has been a 20-year mystery....
Understanding why the glass transition temperature (Tg ) of polymers deviates substantially from the bulk with nanoscale confinement has been a 20-year...
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StartPage 288
SubjectTerms Chain adsorption
Confinement
Decoupling
Dynamic tests
Dynamics
Free volume
Glass transition
Glassy
Polymer thin films
Polymers
Thin films
Title On the equivalence between the thermodynamic and dynamic measurements of the glass transition in confined polymers
URI https://dx.doi.org/10.1016/j.jnoncrysol.2014.09.048
https://search.proquest.com/docview/1660073228
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