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Updated: Jul 5, 2026

Spatial Separation of Molecular Conformers and Clusters
Published on: January 9, 2014
Residual multiparticle entropy does not generally change sign near freezing
William P Krekelberg1, Vincent K Shen, Jeffrey R Errington
1Department of Chemical Engineering, University of Texas at Austin, Austin, Texas 78712-0231, USA. krekel@che.utexas.edu
Abstract:
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 d-dimensional hard-sphere fluids (d=1-5) 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.
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