The residual multiparticle entropy (RMPE) of two- and three-dimensional fluids changes sign near the freezing line, providing a quasiuniversal “one-phase” rule for the location of the liquid-solid transition. We present new simulation results for -dimensional hard-sphere fluids which show, however, that this freezing criterion fails in other spatial dimensions. The results also call into question the idea that a change in sign of the RMPE implies the emergence of a new kind of local structural order in the fluid.
Residual multiparticle entropy does not generally change sign near freezing
William P. Krekelberg, Vincent K. Shen, Jeffrey R. Errington, Thomas M. Truskett; Residual multiparticle entropy does not generally change sign near freezing. J. Chem. Phys. 28 April 2008; 128 (16): 161101. https://doi.org/10.1063/1.2916697
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