Model Energy Landscapes

Pablo G. Debenedetti, Frank H. Stillinger, M. Scott Shell

Research output: Contribution to journalArticle

35 Scopus citations

Abstract

The multidimensional potential-energy "landscape" formalism offers useful insights into the properties of supercooled liquids and glasses. However, its mathematical fundamentals present formidable subtlety and complexity. In the interests of developing a useful approximation for the statistical mechanics of landscapes, we have developed a simple family of models describing the energy-depth distribution of landscape basins. Our analysis begins with the "Gaussian" model that has been advocated in the recent literature, a physically appealing and thermodynamically rather accurate description that straightforwardly predicts a positive-temperature ideal glass transition. Careful enumeration of low-lying basins reveals however that the Gaussian model requires modification in the form of a logarithmic correction. Consequently, we have carried out algebraic and numerical analyses of a logarithmically modified Gaussian model, including depth dependence of the mean intrabasin vibrational free energy. The logarithmic modification has the effect of eliminating the positive-temperature ideal glass transition of the precursor pure-Gaussian model. Nevertheless, it is sufficiently similar to that unmodified model at and above any kinetic glass transition temperature to be able to represent measurable calorimetric data with reasonable accuracy.

Original languageEnglish (US)
Pages (from-to)14434-14442
Number of pages9
JournalJournal of Physical Chemistry B
Volume107
Issue number51
DOIs
StatePublished - Dec 25 2003

All Science Journal Classification (ASJC) codes

  • Physical and Theoretical Chemistry
  • Surfaces, Coatings and Films
  • Materials Chemistry

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    Debenedetti, P. G., Stillinger, F. H., & Scott Shell, M. (2003). Model Energy Landscapes. Journal of Physical Chemistry B, 107(51), 14434-14442. https://doi.org/10.1021/jp030885b