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Area of Science:

  • Polymer Science
  • Materials Science
  • Physical Chemistry

Background:

  • Near-surface enhanced mobility is observed in glassy polymers, but the characteristic length scales (h_t) vary significantly across studies.
  • Previous research indicates enhanced dynamics originating from the polymer surface, yet the precise nature and origin of these length scales remain unclear.

Purpose of the Study:

  • To investigate the origin of differing length scales associated with near-surface enhanced mobility in glassy polymers.
  • To elucidate the structure and relaxation mechanisms within the mobile surface region of polymer films.

Main Methods:

  • Mechanical relaxations of polystyrene films with thicknesses ranging from 5 nm to 186 μm were studied.
  • Analysis focused on changes in relaxation behavior as a function of film thickness.

Main Results:

  • For films thinner than approximately 1 μm, faster relaxation than the bulk was observed, with relaxation time decreasing below 100 nm.
  • A bulk-like relaxation mode appeared for films thicker than 1 μm, while the fast surface mode extended to approximately 1 μm.
  • The mobile surface region is inhomogeneous, consisting of a distinct nanoscale outer layer and a slower microscale sublayer.

Conclusions:

  • The mobile surface region in glassy polymers is not uniform but comprises at least two distinct layers with different relaxation mechanisms.
  • The observed inhomogeneity explains the wide range of length scales reported in the literature for enhanced polymer dynamics.
  • Understanding these distinct relaxation mechanisms is crucial for accurately interpreting measurements of near-surface mobility.