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Crossover between liquid-like and gas-like behaviour in CH4 at 400 K

Smith, D; Hakeem, M; Parisiades, P; Maynard-Casely, HE; Foster, D; Eden, D; Bull, DJ; Marshall, ARL; Adawi, AM; Howie, R; Sapelkin, A; Brazhkin, VV; Proctor, JE

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Authors

D Smith

M Hakeem

P Parisiades

HE Maynard-Casely

D Foster

D Eden

DJ Bull

ARL Marshall

AM Adawi

R Howie

A Sapelkin

VV Brazhkin



Abstract

We report experimental evidence for a crossover between a liquid-like state and a gas-like state in fluid methane (CH4). This crossover is observed in all of our experiments, up to 397 K temperature; 2.1 times the critical temperature of methane. The crossover has been characterized with both Raman spectroscopy and X-ray diffraction in a number of separate experiments, and confirmed to be reversible. We associate this crossover with the Frenkel line - a recently hypothesized crossover in dynamic properties of fluids extending to arbitrarily high pressure and temperature, dividing the phase diagram into separate regions where the fluid possesses liquid-like and gas-like properties. On the liquid-like side the Raman-active vibration increases in frequency linearly as pressure is increased, as expected due to the repulsive interaction between adjacent molecules. On the gas-like side this competes with the attractive Van der Waal’s potential leading the vibration frequency to decrease as pressure is increased.

Journal Article Type Article
Acceptance Date Oct 12, 2017
Publication Date Nov 9, 2017
Deposit Date Oct 23, 2017
Publicly Available Date Nov 20, 2017
Journal Physical Review E (PRE)
Print ISSN 2470-0045
Electronic ISSN 2470-0053
Publisher American Physical Society
Volume 96
Issue 5
Pages 052113
DOI https://doi.org/10.1103/PhysRevE.96.052113
Publisher URL http://dx.doi.org/10.1103/PhysRevE.96.052113
Related Public URLs https://journals.aps.org/pre/

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Manuscript including supplementary material






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