Residual multiparticle entropy does not generally change sign near freezing

J Chem Phys. 2008 Apr 28;128(16):161101. doi: 10.1063/1.2916697.

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.