DOI: 10.1063/1.2244551. Fragility and thermodynamics in nonpolymeric glass-forming liquids

Fragility and thermodynamics in nonpolymeric glass-forming liquids

10.1063/1.2244551

Crossref journal-article

AIP Publishing

The Journal of Chemical Physics (317)

Abstract

For nonpolymeric supercooled liquids, the empirical correlation m=56TgΔCp(Tg)∕ΔHm provides a reliable means of correlating dynamic and thermodynamic variables. The dynamics are characterized by the fragility or steepness index m and the glass transition temperature Tg, while thermodynamics enter in terms of the heat capacity step ΔCp at Tg and the melting enthalpy ΔHm. The combination of the above correlation with the 2∕3 rule for the Tg∕Tm ratio yields an expression, m=40ΔCp(Tg)∕ΔSm, which was rationalized as the correlation of the thermodynamic and kinetic fragilities. Defining a thermodynamic fragility via ΔCp(Tg)∕ΔSm also reveals that the slopes in Kauzmann’s original ΔS(T)∕ΔSm versus T∕Tm plot reflect the fragility concept [Chem. Rev. 43, 219 (1948)], so long as Tm∕Tg=1.5. For the many liquids whose excess heat capacity is a hyperbolic function of temperature, we deduce that the fragility cannot exceed m=170, unless the Tg∕Tm=2∕3 rule breaks down.

Bibliography

Wang, L.-M., Angell, C. A., & Richert, R. (2006). Fragility and thermodynamics in nonpolymeric glass-forming liquids. The Journal of Chemical Physics, 125(7).

Authors 3

Li-Min Wang (first)
C. Austen Angell (additional)
Ranko Richert (additional)

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Dates

Type	When
Created	19 years ago (Aug. 17, 2006, 6:05 p.m.)
Deposited	2 years ago (July 30, 2023, 11:05 p.m.)
Indexed	1 week, 3 days ago (Aug. 12, 2025, 5:29 p.m.)
Issued	19 years ago (Aug. 18, 2006)
Published	19 years ago (Aug. 18, 2006)
Published Online	19 years ago (Aug. 18, 2006)
Published Print	19 years ago (Aug. 21, 2006)

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BibTeX

@article{Wang_2006, title={Fragility and thermodynamics in nonpolymeric glass-forming liquids}, volume={125}, ISSN={1089-7690}, url={http://dx.doi.org/10.1063/1.2244551}, DOI={10.1063/1.2244551}, number={7}, journal={The Journal of Chemical Physics}, publisher={AIP Publishing}, author={Wang, Li-Min and Angell, C. Austen and Richert, Ranko}, year={2006}, month=aug }

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  "abstract": "<jats:p>For nonpolymeric supercooled liquids, the empirical correlation m=56Tg\u0394Cp(Tg)\u2215\u0394Hm provides a reliable means of correlating dynamic and thermodynamic variables. The dynamics are characterized by the fragility or steepness index m and the glass transition temperature Tg, while thermodynamics enter in terms of the heat capacity step \u0394Cp at Tg and the melting enthalpy \u0394Hm. The combination of the above correlation with the 2\u22153 rule for the Tg\u2215Tm ratio yields an expression, m=40\u0394Cp(Tg)\u2215\u0394Sm, which was rationalized as the correlation of the thermodynamic and kinetic fragilities. Defining a thermodynamic fragility via \u0394Cp(Tg)\u2215\u0394Sm also reveals that the slopes in Kauzmann\u2019s original \u0394S(T)\u2215\u0394Sm versus T\u2215Tm plot reflect the fragility concept [Chem. Rev.\u200843, 219 (1948)], so long as Tm\u2215Tg=1.5. For the many liquids whose excess heat capacity is a hyperbolic function of temperature, we deduce that the fragility cannot exceed m=170, unless the Tg\u2215Tm=2\u22153 rule breaks down.</jats:p>",
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