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Why liquids are fragile.

R Casalini1, C M Roland

  • 1Naval Research Laboratory, Code 6120, Washington, DC 20375-5342, USA. casalini@nrl.navy.mil

Physical Review. E, Statistical, Nonlinear, and Soft Matter Physics
|October 26, 2005
PubMed
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This study reveals a linear relationship between liquid fragilities under constant pressure (mP) and constant volume (mV) conditions. This finding highlights how temperature and density jointly influence the dynamics of glass-forming liquids near their glass transition temperature.

Area of Science:

  • Materials Science
  • Physical Chemistry
  • Condensed Matter Physics

Background:

  • Fragility is a key property of glass-forming liquids, describing the temperature dependence of their dynamics.
  • Understanding the interplay between temperature and density effects on relaxation dynamics is crucial for materials science.

Purpose of the Study:

  • To compare the fragilities of glass-forming liquids and polymers under isobaric and isochoric conditions.
  • To establish a quantitative relationship between pressure-dependent (mP) and volume-dependent (mV) fragilities.
  • To elucidate the role of temperature and density in controlling dynamics near the glass transition.

Main Methods:

  • Comparative analysis of fragility (T(g)-normalized temperature dependence of alpha-relaxation times) for 33 glass-forming liquids and polymers.

Related Experiment Videos

  • Experimental conditions included isobaric (constant pressure) and isochoric (constant volume) measurements.
  • Statistical analysis to determine the correlation between mP and mV fragilities.

    • Main Results:

    • A linear correlation was found between isobaric fragility (mP) and isochoric fragility (mV): mP = (37+/-3) + (0.84+/-0.05)mV.
    • The ratio mV/mP quantifies the relative influence of temperature versus density on relaxation dynamics.
    • Strong glass formers exhibit significant density contributions, while fragile liquids are more temperature-activated.

    Conclusions:

    • The fragility of glass-forming liquids is a direct consequence of the interplay between temperature and density effects.
    • The established linear correlation provides a new framework for understanding and predicting liquid dynamics.
    • The findings offer a physical interpretation rooted in intermolecular potentials and scaling laws.