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Correlating fragility and heterogeneous dynamics in polystyrene through single molecule studies.

Alyssa S Manz1, Mariam Aly1, Laura J Kaufman1

  • 1Department of Chemistry, Columbia University, New York, New York 10027, USA.

The Journal of Chemical Physics
|September 1, 2019
PubMed
Summary

Higher molecular weight polymers exhibit increased fragility and dynamic heterogeneity near their glass transition temperature. Single molecule measurements reveal a correlation between molecular weight, fragility, and dynamic heterogeneity in polystyrene.

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Area of Science:

  • Polymer Science
  • Materials Science
  • Physical Chemistry

Background:

  • Macroscopic polymer properties, such as glass transition temperature, are influenced by molecular weight.
  • Polymers near their glass transition exhibit molecular weight-dependent fragility and dynamic heterogeneity.
  • Existing research links molecular weight to fragility but lacks clarity on its connection to dynamic heterogeneity.

Purpose of the Study:

  • To investigate the impact of molecular weight on the degree of dynamic heterogeneity in polystyrene.
  • To explore correlations between molecular weight, fragility, and dynamic heterogeneity near the glass transition temperature.

Main Methods:

  • Utilized single molecule rotational measurements.
  • Embedded two types of fluorescent probes in polystyrene films.
  • Studied polystyrene samples with molecular weights ranging from 0.6 to 1364.0 kg mol⁻¹.

Main Results:

  • Found a correlation between polystyrene molecular weight, fragility, and the degree of dynamic heterogeneity.
  • Observed this correlation through single molecule stretching exponents.
  • Did not find a clear correlation with time scales of dynamic exchange.

Conclusions:

  • Polystyrene molecular weight significantly influences its dynamic heterogeneity and fragility near the glass transition temperature.
  • Single molecule measurements provide insights into the relationship between molecular architecture and polymer dynamics.
  • Further research may be needed to understand the role of dynamic exchange time scales.