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We comment on three incorrect claims in the paper by Fomin et al (arXiv:1507.06094) concerning the generalized hydrodynamic methodology and positive sound dispersion in fluids.
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We comment on an expression for positive sound dispersion (PSD) in fluids and analysis of PSD from molecular dynamics simulations reported in the Letter by Fomin et al (J.Phys.:Condens.Matt. v.28, 43LT01, 2016)
The acoustic sound dispersion of nitrogen in its liquid and supercritical phases has been studied by Inelastic X-Ray Scattering. Approaching supercritical conditions, the gradual disappearance of the positive sound dispersion, characteristic of the low temperature liquid, is observed. In the supercritical state, evidence for a crossover between adiabatic and isothermal sound propagation regimes is inferred by an analysis of the dynamic structure factor based on generalized hydrodynamics.
In a recent paper, S. Singh and K. Tankeshwar (ST), [Phys. Rev. E textbf{67}, 012201 (2003)], proposed a new interpretation of the collective dynamics in liquid metals, and, in particular, of the relaxation mechanisms ruling the density fluctuations propagation. At variance with both the predictions of the current literature and the results of recent Inelastic X-ray Scattering (IXS) experiments, ST associate the quasielastic component of the $S(Q,omega)$ to the thermal relaxation, as it holds in an ordinary adiabatic hydrodynamics valid for non-conductive liquids and in the $Q to 0$ limit. We show here that this interpretation leads to a non-physical behaviour of different thermodynamic and transport parameters.
A hallmark of a thermodynamic phase transition is the qualitative change of system thermodynamic properties such as energy and heat capacity. On the other hand, no phase transition is thought to operate in the supercritical state of matter and, for this reason, it was believed that supercritical thermodynamic properties vary smoothly and without any qualitative changes. Here, we perform extensive molecular dynamics simulations in a wide temperature range and find that a deeply supercritical state is thermodynamically heterogeneous, as witnessed by different temperature dependence of energy, heat capacity and its derivatives at low and high temperature. The evidence comes from three different methods of analysis, two of which are model-independent. We propose a new definition of the relative width of the thermodynamic crossover and calculate it to be in the fairly narrow relative range of 13-20%. On the basis of our results, we relate the crossover to the supercritical Frenkel line.
Physics of supercritical state is understood to a much lesser degree compared to subcritical liquids. Carbon dioxide in particular has been intensely studied, yet little is known about the supercritical part of its phase diagram. Here, we combine neutron scattering experiments and molecular dynamics simulations and demonstrate the structural crossover at the Frenkel line. The crossover is seen at pressures as high as 14 times the critical pressure and is evidenced by changes of the main features of the structure factor and pair distribution functions.
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