Simulating Local Tg Reporting Layers in Glassy Thin Films

Jeffrey DeFelice, Scott T. Milner, Jane E.G. Lipson

Research output: Contribution to journalArticle

17 Scopus citations

Abstract

One of the most notable deviations from bulk fluid properties is the onset of a thickness-dependent glass transition temperature (Tg) for nanometrically thin polymer films. Experimental and theoretical observations suggest that this behavior is a response to the interfaces, which perturb the local properties of a film and play an increasingly important role in influencing the global properties of a film as its thickness decreases. In this work, we probe the global and local properties of free-standing films using our limited mobility (LM) model, which is a simple kinetic lattice model that simulates free volume and mobility in a fluid. We provide insight about the role of mobility in affecting the thickness-dependent film-average Tg of free-standing polymer films by characterizing the depth to which mobility propagates from a free surface, i.e., the "mobile layer depth". We also consider the effect of "stacking" free-standing polymer films, where confinement by interfaces composed of the same material yields Tg suppression intermediate to that of substrate supported and free-standing films. In order to characterize the local properties of a film, we utilize "reporting layers" located near the free surface and film interior, from which we compute local glass transition temperatures and make connections with experimental results reported for real polymer films.

Original languageEnglish (US)
Pages (from-to)1822-1833
Number of pages12
JournalMacromolecules
Volume49
Issue number5
DOIs
StatePublished - Mar 9 2016

All Science Journal Classification (ASJC) codes

  • Organic Chemistry
  • Polymers and Plastics
  • Inorganic Chemistry
  • Materials Chemistry

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