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Comment on “Heat capacity, enthalpy fluctuations, and configurational entropy in broken ergodic systems” [J. Chem. Phys.133, 164503 (2010)]
18. N. G. McCrum, B. E. Read, and G. Williams, Anelastic and Dielectric Effects in Polymeric Solids (Wiley, New York, 1967).
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27.See papers published in special issues on Calorimetry in Thermochim. Acta 304–305 (1997) and 377 (2001).
35. Y. Kraftmakher, Modulation Calorimetry: Theory and Applications (Springer, Berlin, 2004).
36.See chapters in Modulated Temperature Differential Scanning Calorimetry: Theoretical and Practical Applications in Polymer Characterization, edited by M. Reading and D. J. Hourston (Springer, Berlin, 2006).
41. S. L. Simon and G. B. McKenna, J. Chem. Phys. 107, 8678 (1997). The authors showed that Cp′ and Cp′′ spectra can be produced by a simulation based on the Tool–Narayanaswami–Moynihan (TNM) model for structural relaxation that is used to fit the DSC scans. After the discussion meeting on the subject (see Ref. 27 for Proceedings), it was accepted that Cp′ for slow cooling and heating rates show dispersion in the classical sense of compliance within the fluctuation-dissipation theorem, as well as the irreversible changes as in the TNM model. Specific details of this discussion have appeared in Refs. 29 and 30, and 33, and general details in Refs. 20–36.
43. T. A. Litovitz and C. M. Davis, “Structural and shear relaxation in liquids,” in Physical Acoustics, edited by W. P. Mason (Academic, New York, 1965), Vol. II A, pp. 281–349.
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A critical examination shows that the specific heat and shear modulusrelaxation spectra do not support the notions of continuously broken ergodicity and loss of configurational contribution on isothermal glass transition, nor does the long-known result that C p → 0 as T → 0 K prove that S conf → 0. Spectra show variation of the real and imaginary components due to phase lag and not due to loss of configurational degrees of freedom. The high-frequency shear modulus,G ∞, of glass increases with time as its fictive temperature decreases and dG ∞/dT decreases when a glass forms.
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