Quasi-equilibrium phase coexistence in single component supercritical fluids

Seungtaek Lee, Juho Lee, Yeonguk Kim, Seokyong Jeong, Dong Eon Kim () and Gunsu Yun ()
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Seungtaek Lee: Pohang University of Science and Technology
Juho Lee: Pohang University of Science and Technology
Yeonguk Kim: Pohang University of Science and Technology
Seokyong Jeong: Pohang University of Science and Technology
Dong Eon Kim: Pohang University of Science and Technology
Gunsu Yun: Pohang University of Science and Technology

Nature Communications, 2021, vol. 12, issue 1, 1-7

Abstract: Abstract In their supercritical state simple fluids are generally thought to assume a homogeneous phase throughout all combinations of pressures and temperatures, although various response functions or transport properties may exhibit anomalous behavior, characterizing a state point as either more gas-like or liquid-like, respectively. While a large body of results has been compiled in the last two decades regarding the details of the supercritical phase in thermodynamic equilibrium, far less studies have been dedicated to out-of-equilibrium situations that nevertheless occur along with the handling of substances such as carbon dioxide or Argon. Here we consider successive compression-expansion cycles of equal amounts of Argon injected into a high-pressure chamber, traversing the critical pressure at two times the critical temperature. Due to expansion cooling, the fluid temporarily becomes sub-critical, and light scattering experiments show the formation of sub-micron-sized droplets and nanometer-scale clusters, both of which are distinct from spontaneous density fluctuations of the supercritical background and persist for a surprisingly long time. A kinetic rate model of the exchange of liquid droplets with the smaller clusters can explain this behavior. Our results indicate non-equilibrium aspects of supercritical fluids that may prove important for their processing in industrial applications.

Date: 2021
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DOI: 10.1038/s41467-021-24895-y

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