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Segmental relaxations have macroscopic consequences in glassy polymer films

We have investigated the consequences of physical aging in thin spin-coated glassy polystyrene films through detailed dewetting studies. A simultaneous and equally fast exponential decay of dewetting velocity, width, and height of the rim with aging time was observed, which is related to a reduction...

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Main Authors: Chowdhury, Mithun (Author) , Freyberg, Paul (Author) , Ziebert, Falko (Author) , Yang, Arnold C.-M. (Author) , Steiner, Ullrich (Author) , Reiter, Günter (Author)
Format: Article (Journal)
Language:English
Published: 27 September 2012
In: Physical review letters
Year: 2012, Volume: 109, Issue: 13, Pages: 1-5
ISSN:1079-7114
DOI:10.1103/PhysRevLett.109.136102
Online Access:Verlag, lizenzpflichtig, Volltext: https://doi.org/10.1103/PhysRevLett.109.136102
Verlag, lizenzpflichtig, Volltext: https://link.aps.org/doi/10.1103/PhysRevLett.109.136102
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Author Notes:Mithun Chowdhury, Paul Freyberg, Falko Ziebert, Arnold C.-M. Yang, Ullrich Steiner, and Günter Reiter

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520 |a We have investigated the consequences of physical aging in thin spin-coated glassy polystyrene films through detailed dewetting studies. A simultaneous and equally fast exponential decay of dewetting velocity, width, and height of the rim with aging time was observed, which is related to a reduction of residual stresses within such films. The temperature dependence of these decay times followed an Arrhenius behavior, yielding an activation energy of 70±6 kJ/mol, on the same order of magnitude as values for the β-relaxation of polystyrene and for relaxations of surface topographical features. Our results suggest that rearrangements at the level of chain segments are sufficient to partially relax frozen-in out-of-equilibrium local chain conformations, i.e., the cause of residual stresses, and they might also be responsible for macroscopic relaxations at polymer surfaces. 
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