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A Second Glass Transition Observed in Single-Component Homogeneous Liquids Due to Intramolecular Vitrification.

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Area of Science:

  • Physical Chemistry
  • Materials Science
  • Condensed Matter Physics

Background:

  • Supercooling liquids leads to a glass transition, forming an amorphous solid with reduced heat capacity.
  • Pure homogeneous liquids are generally expected to exhibit only a single glass transition.
  • Conventional glass transitions involve the dynamic arrest of bulk liquid properties.

Purpose of the Study:

  • To investigate the glass transition behavior of single-component homogeneous molecular liquids.
  • To determine if multiple glass transitions can occur in such systems.
  • To elucidate the nature of distinct glass transitions observed in titanium tetraalkoxides.

Main Methods:

  • Calorimetric measurements were performed on a family of titanium tetraalkoxides.
  • Analysis focused on identifying and characterizing distinct changes in heat capacity.
  • The study correlated thermal events with molecular dynamics and structural changes.

Main Results:

  • Titanium tetraalkoxides display two calorimetric glass transitions of comparable magnitude.
  • One transition corresponds to the conventional bulk liquid dynamic arrest.
  • The second transition is attributed to the freezing out of intramolecular degrees of freedom.

Conclusions:

  • A novel phenomenon of intramolecular vitrification was observed in homogeneous molecular liquids.
  • This suggests that intramolecular motions can undergo a glass transition independent of bulk properties.
  • Intramolecular barrier-crossing processes may not always follow Arrhenius behavior and can freeze out at finite temperatures.