Residual multiparticle entropy does not generally change sign near freezing.

Department of Chemical Engineering, University of Texas at Austin, Austin, Texas 78712-0231, USA. krekel@che.utexas.edu

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.

PMID: 18447412 [PubMed]