Comment on "Residual multiparticle entropy does not generally change sign near freezing" [J. Chem. Phys. 128, 161101 (2008)].
Does the vanishing of the residual multiparticle entropy, a quantity defined as the cumulative contribution of more-than-two-particle density correlations to the excess entropy of a fluid, have physical significance? We address this question in the light of the arguments presented in the paper that is being commented on and of the phenomenology thus far explored in a variety of model systems undergoing thermodynamic or structural transformations into more ordered (but not necessarily crystalline) states or regimes.
Giaquinta
Paolo V
PV
Dipartimento di Fisica, Universita degli Studi di Messina, Contrada Papardo, 98166 Messina, Italy. paolo.giaquinta@unime.it