DOI: 10.1063/1.2390710. Entropy, diffusivity, and structural order in liquids with waterlike anomalies

Entropy, diffusivity, and structural order in liquids with waterlike anomalies

10.1063/1.2390710

Crossref journal-article

AIP Publishing

The Journal of Chemical Physics (317)

Abstract

The excess entropy, defined as the difference between the entropies of the liquid and the ideal gas under identical density and temperature conditions, is studied as a function of density and temperature for liquid silica and a two-scale ramp potential, both of which are known to possess waterlike liquid state anomalies. The excess entropy for both systems is evaluated using a fairly accurate pair correlation approximation. The connection between the excess entropy and the density and diffusional anomalies is demonstrated. Using the pair correlation approximation to the excess entropy, it can be shown that if the energetically favorable local geometries in the low and high density limits have different symmetries, then a structurally anomalous regime can be defined in terms of orientational and translational order parameters, as in the case of silica and the two-scale ramp system but not for the one-scale ramp liquid. Within the category of liquids with waterlike anomalies, we show that the relationship between the macroscopic entropy and internal energy is sufficient to distinguish between those with local anisotropy and consequent open packings at low densities and those with isotropic interactions but multiple length scales. Since it is straightforward to evaluate the pair correlation entropy and internal energy from simulations or experimental data, such plots should provide a convenient means to diagnose the existence as well as type of anomalous behavior in a range of liquids, including ionic and intermetallic melts and complex fluids with ultrasoft repulsions.

Bibliography

Sharma, R., Chakraborty, S. N., & Chakravarty, C. (2006). Entropy, diffusivity, and structural order in liquids with waterlike anomalies. The Journal of Chemical Physics, 125(20).

Authors 3

Ruchi Sharma (first)
Somendra Nath Chakraborty (additional)
Charusita Chakravarty (additional)

References 59 Referenced 179

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Dates

Type	When
Created	18 years, 9 months ago (Nov. 22, 2006, 6:18 p.m.)
Deposited	2 years ago (July 31, 2023, 10:17 p.m.)
Indexed	2 weeks, 2 days ago (Aug. 6, 2025, 9:49 a.m.)
Issued	18 years, 9 months ago (Nov. 22, 2006)
Published	18 years, 9 months ago (Nov. 22, 2006)
Published Online	18 years, 9 months ago (Nov. 22, 2006)
Published Print	18 years, 8 months ago (Nov. 28, 2006)

Funders 0

None

BibTeX

@article{Sharma_2006, title={Entropy, diffusivity, and structural order in liquids with waterlike anomalies}, volume={125}, ISSN={1089-7690}, url={http://dx.doi.org/10.1063/1.2390710}, DOI={10.1063/1.2390710}, number={20}, journal={The Journal of Chemical Physics}, publisher={AIP Publishing}, author={Sharma, Ruchi and Chakraborty, Somendra Nath and Chakravarty, Charusita}, year={2006}, month=nov }

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