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A free-energy landscape picture and Landau theory for the dynamics of disordered materials
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10.1063/1.2354471
/content/aip/journal/jcp/125/15/10.1063/1.2354471
http://aip.metastore.ingenta.com/content/aip/journal/jcp/125/15/10.1063/1.2354471
View: Figures

Figures

Image of FIG. 1.
FIG. 1.

Sketch of internal energy (solid curve) and grand potential per particle (broken curves) as a function of the dynamical order parameter . Quantitative values, from the fit to glycerol shown in Fig. 2, correspond to room temperature, the glass transition, and from top to bottom, respectively. The internal-energy minima occur at , but if the free-energy minimum is at . For a fixed free-energy curvature, normal thermal fluctuations about increase with increasing temperature, canceling the explicit temperature dependence in the Arrhenius law to give approximate time-temperature superposition. However, the thermal fluctuations and average potential-energy barrier tend to diverge as the curvature goes to zero at , yielding VTF-type behavior. The normal thermal fluctuations also increase with decreasing system size, so that subdividing a system into smaller regions lowers the net internal energy.

Image of FIG. 2.
FIG. 2.

Angell plot of the characteristic relaxation time as a function of inverse temperature. The symbols are from the measured peak dielectric loss of (엯) glycerol and (◻) propylene glycol from Ref. 39. The solid curves are from fits to the data using a fourth-order approximation of the free energy to obtain the temperature-dependent activation energy, , as described in the text.

Image of FIG. 3.
FIG. 3.

Log-log plot of the frequency-dependent response of glycerol at four temperatures. The symbols are from measurements of dielectric loss from Ref. 40. The solid curves are from fits to the data using a distribution of sizes and size-dependent relaxation time , as described in the text.

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/content/aip/journal/jcp/125/15/10.1063/1.2354471
2006-10-18
2014-04-24
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752b84549af89a08dbdd7fdb8b9568b5 journal.articlezxybnytfddd
Scitation: A free-energy landscape picture and Landau theory for the dynamics of disordered materials
http://aip.metastore.ingenta.com/content/aip/journal/jcp/125/15/10.1063/1.2354471
10.1063/1.2354471
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