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Title: Two-component dynamics and the liquid-like to gas-like crossover in supercritical water

Abstract

Molecular-scale dynamics in sub- to supercritical water is studied with inelastic x-ray scattering and molecular dynamics simulations. The obtained longitudinal current correlation spectra can be decomposed into two main components: a low-frequency (LF), gaslike component and a high-frequency (HF) component arising from the O-O stretching mode between hydrogen-bonded molecules, reminiscent of the longitudinal acoustic mode in ambient water. With increasing temperature, the hydrogen-bond network diminishes and the spectral weight shifts from HF to LF, leading to a transition from liquid- to gaslike dynamics with rapid changes around the Widom line.

Authors:
ORCiD logo [1];  [2]; ORCiD logo [3]; ORCiD logo [3];  [4]
+ Show Author Affiliations
  1. SLAC National Accelerator Lab., Menlo Park, CA (United States); Stanford Univ., CA (United States)
  2. SLAC National Accelerator Lab., Menlo Park, CA (United States)
  3. RIKEN SPring-8 Center, Sayo (Japan). Materials Dynamics Lab.
  4. Univ. di Trento (Italy)
Publication Date:
Research Org.:
SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1712673
Alternate Identifier(s):
OSTI ID: 1735570
Grant/Contract Number:  
AC02-76SF00515
Resource Type:
Accepted Manuscript
Journal Name:
Physical Review Letters
Additional Journal Information:
Journal Volume: 125; Journal Issue: 25; Journal ID: ISSN 0031-9007
Publisher:
American Physical Society (APS)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Sun, Peihao, Hastings, Jerome B., Ishikawa, Daisuke, Baron, Alfred Q. R., and Monaco, Giulio. Two-component dynamics and the liquid-like to gas-like crossover in supercritical water. United States: N. p., 2020. Web. doi:10.1103/PhysRevLett.125.256001.
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Sun, Peihao, Hastings, Jerome B., Ishikawa, Daisuke, Baron, Alfred Q. R., & Monaco, Giulio. Two-component dynamics and the liquid-like to gas-like crossover in supercritical water. United States. https://doi.org/10.1103/PhysRevLett.125.256001
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Sun, Peihao, Hastings, Jerome B., Ishikawa, Daisuke, Baron, Alfred Q. R., and Monaco, Giulio. Sun . "Two-component dynamics and the liquid-like to gas-like crossover in supercritical water". United States. https://doi.org/10.1103/PhysRevLett.125.256001. https://www.osti.gov/servlets/purl/1712673.
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@article{osti_1712673,
title = {Two-component dynamics and the liquid-like to gas-like crossover in supercritical water},
author = {Sun, Peihao and Hastings, Jerome B. and Ishikawa, Daisuke and Baron, Alfred Q. R. and Monaco, Giulio},
abstractNote = {Molecular-scale dynamics in sub- to supercritical water is studied with inelastic x-ray scattering and molecular dynamics simulations. The obtained longitudinal current correlation spectra can be decomposed into two main components: a low-frequency (LF), gaslike component and a high-frequency (HF) component arising from the O-O stretching mode between hydrogen-bonded molecules, reminiscent of the longitudinal acoustic mode in ambient water. With increasing temperature, the hydrogen-bond network diminishes and the spectral weight shifts from HF to LF, leading to a transition from liquid- to gaslike dynamics with rapid changes around the Widom line.},
doi = {10.1103/PhysRevLett.125.256001},
journal = {Physical Review Letters},
number = 25,
volume = 125,
place = {United States},
year = {Sun Oct 04 00:00:00 EDT 2020},
month = {Sun Oct 04 00:00:00 EDT 2020}
}
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https://doi.org/10.1103/PhysRevLett.125.256001
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