2020
DOI: 10.1103/physreve.101.052109
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Experimental and modeling evidence for structural crossover in supercritical CO2

Abstract: The physics of supercritical states 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 … Show more

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Cited by 16 publications
(10 citation statements)
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References 45 publications
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“…Guided by theoretical prediction, subsequent experiments have confirmed the transition at the Frenkel line in supercritical Ne [52], CH 4 [53], N 2 [54], C 2 H 6 [55] and CO 2 [56] using X-ray, neutron and Raman scattering techniques.…”
Section: Dynamical Crossover At the Frenkel Linementioning
confidence: 88%
“…Guided by theoretical prediction, subsequent experiments have confirmed the transition at the Frenkel line in supercritical Ne [52], CH 4 [53], N 2 [54], C 2 H 6 [55] and CO 2 [56] using X-ray, neutron and Raman scattering techniques.…”
Section: Dynamical Crossover At the Frenkel Linementioning
confidence: 88%
“…This allowed authors in Ref. [71] to perform statistical analysis, which decisively confirmed a crossover in the functional dependence of r/r 0 on (V /V 0 ) 1/3 . In this sense the NS data corroborate the structural crossover in real space, rather than unequivocally demonstrating it alone.…”
Section: Carbon Dioxidementioning
confidence: 77%
“…The proportionality constant will depend on the system's structure and on the existence of more condensed phases at higher densities (see Ref. [71] for a detailed discussion). If, on the other hand, the system's structure changes due to coordination rearrangements or a change in orientation order, for example, r fnn will experience changes from more sources than just the change in density, and will therefore not be proportional to V 1/3 .…”
Section: Carbon Dioxidementioning
confidence: 99%
“…This disappearance of transverse modes and the condition c V = 2 correspond to the Frenkel line, which separates two dynamical regimes of particle motion: combined oscillatory and diffusive motion in the low-temperature "rigid" liquid (rigid in a sense of its ability to support solid-like transverse modes); and purely diffusive motion in the high-temperature non-rigid gaslike fluid [12]. Experimentally, the transitions at the Frenkel line have been observed in supercritical Ne [21], CH 4 [22], N 2 [23], C 2 H 6 [24] and CO 2 [25] using X-ray, neutron and Raman scattering techniques.…”
Section: Resultsmentioning
confidence: 99%