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Evidence for structural crossover in the supercritical state.

Dima Bolmatov1, V V Brazhkin2, Yu D Fomin2

  • 1Baker Laboratory, Cornell University, Ithaca, New York 14853-1301, USA.

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|December 24, 2013
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Supercritical fluids are not featureless. A structural crossover reveals distinct liquid-like and gas-like states, linking structure, dynamics, and thermodynamics in this poorly understood state of matter.

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Area of Science:

  • Thermodynamics
  • Materials Science
  • Physical Chemistry

Background:

  • The supercritical state, matter above its critical point, is often considered homogeneous.
  • Current understanding suggests gradual, featureless property changes with pressure and temperature in supercritical fluids.
  • The structure of supercritical fluids is assumed to be uniform across the phase diagram.

Purpose of the Study:

  • To challenge the view of a featureless supercritical state.
  • To identify and characterize structural changes within the supercritical fluid phase diagram.
  • To investigate the relationship between supercritical structure, dynamics, and thermodynamics.

Main Methods:

  • Analysis of distribution functions for interatomic distances and angles.
  • Qualitative assessment of structural configurations.
  • Correlation analysis between structural, dynamic, and thermodynamic properties.

Main Results:

  • Demonstrated a well-defined structural crossover in supercritical fluids.
  • Identified distinct liquid-like and gas-like configurations.
  • Observed medium-range structural correlations.
  • Linked the structural crossover to known dynamic and thermodynamic crossovers.

Conclusions:

  • The supercritical state exhibits a defined structural crossover, not a gradual featureless change.
  • This crossover separates liquid-like and gas-like structural behaviors.
  • New fundamental connections between supercritical structure, dynamics, and thermodynamics are revealed.