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Connectivity and free-surface effects in polymer glasses.

Anna Lappala1,2, Luke Sefton3,4, Paul W Fenimore5

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Polymer glass dynamics depend on particle connections, not chain sequence, in bulk. Surface effects differ, showing distinct behavior near the free surface.

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Area of Science:

  • Condensed matter physics
  • Materials science
  • Polymer physics

Background:

  • The glass transition remains an unsolved problem in condensed matter physics.
  • Glasses are amorphous solids with arrested dynamics, lacking long-range crystalline order.
  • Polymer glasses may differ fundamentally from standard glass-formers due to connectivity.

Purpose of the Study:

  • To investigate the role of connectivity in polymer glass formation and dynamics.
  • To determine if polymer chain sequentiality is critical for bulk glassy dynamics.
  • To differentiate between bulk and surface effects in polymer glasses.

Main Methods:

  • Analysis of connectivity in polymer glasses.
  • Comparison of bulk and surface dynamics in model coarse-grained polymer chains.
  • Application of Phillips-Thorpe topological constraint theory.

Main Results:

  • Bulk glassy dynamics depend on the number of connections per particle, not bonding sequentiality.
  • Covalent bonding promotes glass formation, but chain sequence is not critical in the bulk.
  • Bonding sequentiality significantly influences surface effects, distinguishing polymer from colloidal glasses.
  • Heterogeneous dynamics and domain patterns were identified in polymer chains near the surface.

Conclusions:

  • Glassy dynamics in bulk polymers are governed by topological constraints (number of connections), aligning with Phillips-Thorpe theory.
  • Polymer chain sequentiality is crucial for surface properties but not bulk dynamics.
  • A key difference exists between polymeric and colloidal glasses regarding surface effects.