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Toward a density-functional theory for the Jagla fluid.

Florian Gußmann1,2, S Dietrich2,3, Roland Roth1

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Area of Science:

  • Thermodynamics
  • Statistical Mechanics
  • Computational Physics

Background:

  • The Jagla fluid models water's unique properties, including a liquid-liquid critical point and density anomaly.
  • Experimental verification of water's liquid-liquid critical point is hindered by crystallization in supercooled states.

Purpose of the Study:

  • To model the inhomogeneous Jagla fluid using classical density-functional theory (DFT).
  • To understand how confinement influences the Jagla fluid's phase behavior.
  • To potentially guide experimental tests for water's liquid-liquid critical point.

Main Methods:

  • Determined the Jagla fluid's bulk phase diagram using thermodynamical perturbation theory.
  • Investigated the limitations of existing perturbation theories for the Jagla fluid.
  • Constructed a perturbative DFT model, improving upon standard mean-field DFT.

Main Results:

  • The perturbative DFT showed improvement over mean-field DFT for the Jagla fluid.
  • Existing perturbation theories were found to be inadequate for describing the Jagla fluid.
  • The developed perturbative DFT failed near the binodal line and at low temperatures.

Conclusions:

  • The perturbative DFT approach has limitations for modeling the Jagla fluid under specific conditions.
  • The study could not achieve the goal of simulating highly confined Jagla fluid near its liquid-liquid critical point.
  • Further theoretical development is needed to accurately model inhomogeneous Jagla fluid behavior.