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Universal Two-Component Dynamics in Supercritical Fluids.

Peihao Sun1,2, J B Hastings1, Daisuke Ishikawa3

  • 1SLAC National Accelerator Laboratory, 2575 Sand Hill Road, Menlo Park, California 94025, United States.

The Journal of Physical Chemistry. B
|December 2, 2021
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Summary
This summary is machine-generated.

Supercritical fluids exhibit universal two-component dynamics, transitioning from liquidlike to gaslike behavior. This transition, driven by component ratios, reveals insights into fluid properties and microscopic mechanisms.

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Area of Science:

  • Physical Chemistry
  • Materials Science
  • Computational Physics

Background:

  • Supercritical fluids are technologically important but their microscopic dynamics remain poorly understood.
  • Existing models struggle to fully explain the complex behavior of these states of matter.

Purpose of the Study:

  • To investigate the microscopic intermolecular dynamics of various supercritical fluid systems.
  • To identify universal behaviors and underlying mechanisms governing supercritical fluid dynamics.

Main Methods:

  • Classical molecular dynamics simulations were employed.
  • Four distinct systems were studied: supercritical water, silicon (Si), tellurium (Te), and a Lennard-Jones fluid.
  • Analysis focused on the intermolecular dynamics and their relationship to thermodynamic properties.

Main Results:

  • A universal two-component behavior was observed across all simulated supercritical fluids.
  • A crossover from liquidlike to gaslike dynamics was identified, most pronounced near the Widom line.
  • The ratio of the two dynamic components correlates with fluid properties like self-diffusion coefficients.
  • Liquidlike dynamics are linked to intermolecular bonding, while gaslike dynamics relate to free-particle motion.

Conclusions:

  • The study reveals a fundamental, universal mechanism controlling supercritical fluid dynamics.
  • Spatiotemporally inhomogeneous dynamics play a crucial role, even in the absence of large-scale fluctuations.
  • The findings offer a new perspective on understanding and predicting supercritical fluid behavior.