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Fragility and Tendency to Crystallization for Structurally Related Compounds.

Katarzyna Grzybowska1, Zaneta Wojnarowska1, Andrzej Grzybowski1

  • 1Institute of Physics, University of Silesia in Katowice, ul. 75 Pulku Piechoty 1, 41-500 Chorzów, Poland.

International Journal of Molecular Sciences
|March 28, 2024
PubMed
Summary

Three organic materials with similar structures showed distinct crystallization behaviors. Dynamic fragility did not predict crystallization tendency, but thermodynamic fragility did, highlighting its importance in material science.

Keywords:
amorphous materialscrystallizationfragilityglass transitionmolecular dynamicsphysical stabilitysupercooled liquidthermodynamic fragility

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Area of Science:

  • Materials Science
  • Physical Chemistry
  • Solid State Physics

Background:

  • Investigating the physical stability of organic materials is crucial for understanding their behavior in supercooled liquid states.
  • Similar chemical structures can exhibit vastly different crystallization tendencies.
  • Understanding factors influencing crystallization is key for designing stable materials.

Purpose of the Study:

  • To investigate the physical stability and crystallization tendencies of three organic materials with similar chemical structures.
  • To determine the relationship between dynamic and thermodynamic fragility and crystallization behavior.
  • To classify compounds based on their crystallization propensity from the melt and upon reheating.

Main Methods:

  • Broadband dielectric spectroscopy to study molecular dynamics and structural relaxation.
  • Conventional and temperature-modulated differential scanning calorimetry (DSC) for thermal properties and glass transition analysis.
  • Isothermal crystallization kinetics studies for materials exhibiting crystalline transformation.

Main Results:

  • The three compounds, differing only by oxygen or sulfur in their rings, displayed distinct crystallization behaviors: easy crystallization, crystallization upon reheating, or no crystallization.
  • All glass formers exhibited the same dynamic fragility (m = 93), indicating it is unrelated to crystallization tendency.
  • Thermodynamic fragility, derived from the glass transition width in heat capacity data, showed a strong correlation with crystallization tendency.

Conclusions:

  • Crystallization tendency in supercooled liquids is not dictated by dynamic fragility.
  • Thermodynamic fragility, reflecting the width of the glass transition, is a better predictor of a material's propensity to crystallize.
  • Subtle structural differences (e.g., O vs. S atoms) significantly impact crystallization behavior, despite overall structural similarity.