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Unlike ionic or small covalent molecules, polymers do not form crystalline solids due to the diffusion limitations of their long-chain structures. However, polymers contain microscopic crystalline domains separated by amorphous domains.
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Modeling polymer crystallisation induced by a moving heat sink.

Sabin Adhikari1, Ahana Purushothaman2, Alejandro A Krauskopf1

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

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|January 28, 2021
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Summary

Polymer crystallization can organize nanoparticles. Modeling this, we found that while kinetics don't change the basic physics, increasing zone annealing speed lowers the crystal-melt interface temperature, aligning with theories on undercooling.

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Area of Science:

  • Materials Science
  • Polymer Physics
  • Thermodynamics

Background:

  • Experimental studies demonstrate polymer crystallization's ability to organize nanoparticles.
  • Existing models often assume crystallization at a single temperature, which is an oversimplification for polymers.

Purpose of the Study:

  • To model nanoparticle organization by polymer crystallization.
  • To investigate the physics of directional polymer melt recrystallization using a moving heat sink (zone annealing).
  • To analyze the relationship between heat sink velocity and the crystallization interface temperature.

Main Methods:

  • Adapted the classical Stefan problem to incorporate polymer crystallization kinetics dependent on subcooling, inspired by the Avrami model.
  • Simulated directional recrystallization of a polymer melt using a moving heat sink.
  • Analyzed the steady-state behavior of the solid-melt interface relative to the heat sink.

Main Results:

  • The polymer crystallization front's movement, defined at 50% crystallinity, closely matches the classical Stefan problem, indicating minimal impact of kinetics at this approximation.
  • A steady state was observed for directional recrystallization, with the interface moving at the same velocity as the heat sink.
  • The interface-to-sink distance decreased with increasing sink velocity, and importantly, the crystal-melt interface temperature decreased with higher velocities.

Conclusions:

  • Polymer crystallization kinetics do not qualitatively alter the fundamental physics of nanoparticle movement at the modeled approximation.
  • Directional zone annealing of polymer melts exhibits a steady state where interface temperature decreases with increasing annealing velocity.
  • The findings support theoretical predictions linking higher zone annealing velocities to increased effective undercoolings during polymer crystallization.