Residual Multiparticle Entropy Does Not Generally Change Sign Near Freezing
William P. Krekelberg, Vincent K. Shen, Jeffrey R. Errington, Thomas M. Truskett
The residual multiparticle entropy (RMPE) of two- and three-dimensional fluids changes sign near the freezing line, providing a quasi-universal one-phase rule for the location of the liquid-solid transition. We present new simulation results ford-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.
Journal of Chemical Physics
entropy, freezing, hard hyperspheres, hard spheres, molecular dynamics, Monte Carlo, thermodynamics