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This study reveals dynamic heterogeneity in polymer solutions during stress relaxation. Distinct molecular subpopulations exhibit unique relaxation behaviors, offering insights into polymer dynamics.

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Area of Science:

  • Polymer physics
  • Soft matter science
  • Rheology

Background:

  • Stress relaxation in entangled polymers is crucial for understanding material properties.
  • Transient chain entanglement dynamics significantly influence relaxation processes.
  • The transition from unentangled to entangled states presents complex relaxation behaviors.

Purpose of the Study:

  • To investigate polymer relaxation mechanisms in the transition regime from unentangled to entangled solutions.
  • To identify and characterize dynamic heterogeneity in polymer relaxation.
  • To elucidate the role of transient disentanglement in stress relaxation.

Main Methods:

  • Utilizing single-molecule techniques to probe individual polymer behavior.
  • Analyzing relaxation dynamics across a spectrum of polymer concentrations.
  • Employing multi-exponential fitting to deconvolve distinct relaxation processes.

Main Results:

  • Observed dynamic heterogeneity with distinct molecular subpopulations.
  • Identified single-mode and double-mode exponential relaxation processes.
  • Correlated relaxation timescales with reptation and local disentanglement events.

Conclusions:

  • Dynamic heterogeneity is a key feature of polymer relaxation in the transition regime.
  • Transient disentanglement contributes to distinct relaxation timescales.
  • Single-molecule studies provide critical insights into complex polymer dynamics.