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Segmental Relaxations have Macroscopic Consequences in Glassy Polymer Films

Mithun Chowdhury1,*,†, Paul Freyberg1, Falko Ziebert1,2, Arnold C.-M. Yang3, Ullrich Steiner4,5, and Günter Reiter1,5,‡

  • 1Physikalisches Institut, Albert-Ludwigs-Universität, 79104 Freiburg, Germany
  • 2Institut Charles Sadron UPR22-CNRS, 67034 Strasbourg Cedex 2, France
  • 3Department of Materials Science and Engineering, National Tsing Hua University, Hsinchu, Taiwan
  • 4Cavendish Laboratory, University of Cambridge, Cambridge CB3 0HE, United Kingdom
  • 5Freiburg Institute for Advanced Studies, Albert-Ludwigs-Universität, 79104 Freiburg, Germany

  • *mch.mater@gmail.com
  • †Current address: CRANN and School of Physics, Trinity College, Dublin 2, Ireland
  • ‡guenter.reiter@physik.uni-freiburg.de
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Phys. Rev. Lett. 109, 136102 – Published 27 September, 2012

DOI: https://doi.org/10.1103/PhysRevLett.109.136102

Abstract

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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Phys. Rev. Lett. 109, 136102– Published 27 September, 2012
  • Received 15 June 2012

© 2012 American Physical Society

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