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Universal Two-Component Dynamics in Supercritical Fluids
[Image: see text] Despite the technological importance of supercritical fluids, controversy remains about the details of their microscopic dynamics. In this work, we study four supercritical fluid systems—water, Si, Te, and Lennard-Jones fluid—via classical molecular dynamics simulations. A universa...
Autores principales: | , , , , |
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Formato: | Online Artículo Texto |
Lenguaje: | English |
Publicado: |
American Chemical Society
2021
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Acceso en línea: | https://www.ncbi.nlm.nih.gov/pmc/articles/PMC8686117/ https://www.ncbi.nlm.nih.gov/pubmed/34855409 http://dx.doi.org/10.1021/acs.jpcb.1c07900 |
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author | Sun, Peihao Hastings, J. B. Ishikawa, Daisuke Baron, Alfred Q. R. Monaco, Giulio |
author_facet | Sun, Peihao Hastings, J. B. Ishikawa, Daisuke Baron, Alfred Q. R. Monaco, Giulio |
author_sort | Sun, Peihao |
collection | PubMed |
description | [Image: see text] Despite the technological importance of supercritical fluids, controversy remains about the details of their microscopic dynamics. In this work, we study four supercritical fluid systems—water, Si, Te, and Lennard-Jones fluid—via classical molecular dynamics simulations. A universal two-component behavior is observed in the intermolecular dynamics of these systems, and the changing ratio between the two components leads to a crossover from liquidlike to gaslike dynamics, most rapidly around the Widom line. We find evidence to connect the liquidlike component dominating at lower temperatures with intermolecular bonding and the component prominent at higher temperatures with free-particle, gaslike dynamics. The ratio between the components can be used to describe important properties of the fluid, such as its self-diffusion coefficient, in the transition region. Our results provide an insight into the fundamental mechanism controlling the dynamics of supercritical fluids and highlight the role of spatiotemporally inhomogeneous dynamics even in thermodynamic states where no large-scale fluctuations exist in the fluid. |
format | Online Article Text |
id | pubmed-8686117 |
institution | National Center for Biotechnology Information |
language | English |
publishDate | 2021 |
publisher | American Chemical Society |
record_format | MEDLINE/PubMed |
spelling | pubmed-86861172021-12-21 Universal Two-Component Dynamics in Supercritical Fluids Sun, Peihao Hastings, J. B. Ishikawa, Daisuke Baron, Alfred Q. R. Monaco, Giulio J Phys Chem B [Image: see text] Despite the technological importance of supercritical fluids, controversy remains about the details of their microscopic dynamics. In this work, we study four supercritical fluid systems—water, Si, Te, and Lennard-Jones fluid—via classical molecular dynamics simulations. A universal two-component behavior is observed in the intermolecular dynamics of these systems, and the changing ratio between the two components leads to a crossover from liquidlike to gaslike dynamics, most rapidly around the Widom line. We find evidence to connect the liquidlike component dominating at lower temperatures with intermolecular bonding and the component prominent at higher temperatures with free-particle, gaslike dynamics. The ratio between the components can be used to describe important properties of the fluid, such as its self-diffusion coefficient, in the transition region. Our results provide an insight into the fundamental mechanism controlling the dynamics of supercritical fluids and highlight the role of spatiotemporally inhomogeneous dynamics even in thermodynamic states where no large-scale fluctuations exist in the fluid. American Chemical Society 2021-12-02 2021-12-16 /pmc/articles/PMC8686117/ /pubmed/34855409 http://dx.doi.org/10.1021/acs.jpcb.1c07900 Text en © 2021 The Authors. Published by American Chemical Society https://creativecommons.org/licenses/by/4.0/Permits the broadest form of re-use including for commercial purposes, provided that author attribution and integrity are maintained (https://creativecommons.org/licenses/by/4.0/). |
spellingShingle | Sun, Peihao Hastings, J. B. Ishikawa, Daisuke Baron, Alfred Q. R. Monaco, Giulio Universal Two-Component Dynamics in Supercritical Fluids |
title | Universal Two-Component Dynamics in Supercritical
Fluids |
title_full | Universal Two-Component Dynamics in Supercritical
Fluids |
title_fullStr | Universal Two-Component Dynamics in Supercritical
Fluids |
title_full_unstemmed | Universal Two-Component Dynamics in Supercritical
Fluids |
title_short | Universal Two-Component Dynamics in Supercritical
Fluids |
title_sort | universal two-component dynamics in supercritical
fluids |
url | https://www.ncbi.nlm.nih.gov/pmc/articles/PMC8686117/ https://www.ncbi.nlm.nih.gov/pubmed/34855409 http://dx.doi.org/10.1021/acs.jpcb.1c07900 |
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