Selenium glass transition: A model based on the enthalpy landscape approach and nonequilibrium statistical mechanics

John Mauro, Roger J. Loucks

Research output: Contribution to journalArticle

55 Citations (Scopus)

Abstract

We present a statistical model of the selenium glass transition based on the enthalpy landscape approach and nonequilibrium statistical mechanics. The model offers predictive calculation of the macroscopic properties of a glass-forming system, accounting for the effects of both composition and thermal history. In particular, we compute volume-temperature diagrams for selenium, starting from the equilibrium liquid state and cooling through the glass transition regime. We show excellent agreement between the computed molar volume and thermal expansion coefficient of selenium glass and those measured experimentally by Varshneya and co-workers. Since the model implementation is not limited by time scale, we can achieve realistic cooling rates not accessible to standard molecular simulations. To demonstrate the versatility of our modeling approach, we compute the molar volume of selenium glass with cooling rates ranging from 10-12 to 1012 K/s. The model can also capture thermal compaction (hysteresis) behavior upon subsequent heat treatment of the initially cooled glass. Finally, we present a technique for computation of shear viscosity at and below the glass transition range and apply this technique to selenium. This technique also enables calculation of the fragility of a supercooled liquid.

Original languageEnglish (US)
Article number174202
JournalPhysical Review B - Condensed Matter and Materials Physics
Volume76
Issue number17
DOIs
StatePublished - Nov 9 2007

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Statistical mechanics
Selenium
selenium
statistical mechanics
Glass transition
Enthalpy
enthalpy
glass
Glass
Cooling
Density (specific gravity)
cooling
Shear viscosity
Liquids
Thermal expansion
Hysteresis
Compaction
versatility
Heat treatment
liquids

All Science Journal Classification (ASJC) codes

  • Electronic, Optical and Magnetic Materials
  • Condensed Matter Physics

Cite this

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abstract = "We present a statistical model of the selenium glass transition based on the enthalpy landscape approach and nonequilibrium statistical mechanics. The model offers predictive calculation of the macroscopic properties of a glass-forming system, accounting for the effects of both composition and thermal history. In particular, we compute volume-temperature diagrams for selenium, starting from the equilibrium liquid state and cooling through the glass transition regime. We show excellent agreement between the computed molar volume and thermal expansion coefficient of selenium glass and those measured experimentally by Varshneya and co-workers. Since the model implementation is not limited by time scale, we can achieve realistic cooling rates not accessible to standard molecular simulations. To demonstrate the versatility of our modeling approach, we compute the molar volume of selenium glass with cooling rates ranging from 10-12 to 1012 K/s. The model can also capture thermal compaction (hysteresis) behavior upon subsequent heat treatment of the initially cooled glass. Finally, we present a technique for computation of shear viscosity at and below the glass transition range and apply this technique to selenium. This technique also enables calculation of the fragility of a supercooled liquid.",
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