Bryk T, Gorelli F A, Mryglod I, Ruocco G, Santoro M, Scopigno T
Institute for Condensed Matter Physics of the National Academy of Sciences of Ukraine , 1 Svientsitskii Street, UA-79011 Lviv, Ukraine.
Institute of Applied Mathematics and Fundamental Sciences, Lviv Polytechnic National University , UA-79013 Lviv, Ukraine.
J Phys Chem Lett. 2017 Oct 19;8(20):4995-5001. doi: 10.1021/acs.jpclett.7b02176. Epub 2017 Sep 29.
The "Frenkel line" (FL), the thermodynamic locus where the time for a particle to move by its size equals the shortest transverse oscillation period, has been proposed as a boundary between recently discovered liquid-like and gas-like regions in supercritical fluids. We report a simulation study of isothermal supercritical neon in a range of densities intersecting the FL. Specifically, structural properties and single-particle and collective dynamics are scrutinized to unveil the onset of any anomalous behavior at the FL. We find that (i) the pair distribution function smoothly evolves across the FL displaying medium-range order, (ii) low-frequency transverse excitations are observed below the "Frenkel frequency", and (iii) the high-frequency shear modulus does not vanish even for low-density fluids, indicating that positive sound dispersion characterizing the liquid-like region of the supercritical state is unrelated to transverse dynamics. These facts critically undermine the definition of the FL and its significance for any relevant partition of the supercritical phase.
“弗伦克尔线”(FL)是一个热力学轨迹,在该轨迹上粒子移动自身大小所需的时间等于最短横向振荡周期,它被提议作为超临界流体中最近发现的类液区和类气区之间的边界。我们报告了在一系列与弗伦克尔线相交的密度范围内对等温超临界氖的模拟研究。具体而言,对结构性质以及单粒子动力学和集体动力学进行了仔细研究,以揭示在弗伦克尔线处任何异常行为的起始情况。我们发现:(i)对分布函数在弗伦克尔线上平稳演化,显示出中程有序;(ii)在“弗伦克尔频率”以下观察到低频横向激发;(iii)即使对于低密度流体,高频剪切模量也不会消失,这表明表征超临界态类液区的正声频散与横向动力学无关。这些事实严重削弱了弗伦克尔线的定义及其对超临界相任何相关划分的意义。