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Title: The Frenkel Line: a direct experimental evidence for the new thermodynamic boundary

Abstract

We report that supercritical fluids play a significant role in elucidating fundamental aspects of liquid matter under extreme conditions. They have been extensively studied at pressures and temperatures relevant to various industrial applications. However, much less is known about the structural behaviour of supercritical fluids and no structural crossovers have been observed in static compression experiments in any temperature and pressure ranges beyond the critical point. The structure of supercritical state is currently perceived to be uniform everywhere on the pressure-temperature phase diagram, and to change only in a monotonic way even moving around the critical point, not only along isotherms or isobars. Conversely, we observe structural crossovers for the first time in a deeply supercritical sample through diffraction measurements in a diamond anvil cell and discover a new thermodynamic boundary on the pressure-temperature diagram. We explain the existence of these crossovers in the framework of the phonon theory of liquids using molecular dynamics simulations. The obtained results are of prime importance since they imply a global reconsideration of the mere essence of the supercritical phase. Furthermore, this discovery may pave the way to new unexpected applications and to the exploration of exotic behaviour of confined fluids relevant to geo-more » and planetary sciences.« less

Authors:
 [1];  [1];  [2];  [3];  [1];  [1]
  1. Brookhaven National Lab. (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II)
  2. Volgograd State Technical Univ., Volgograd (Russia)
  3. Univ. of Chicago, IL (United States). Center for Advanced Radiation Sources (CARS)
Publication Date:
Research Org.:
Argonne National Lab. (ANL), Argonne, IL (United States). Advanced Photon Source (APS)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1235468
Grant/Contract Number:  
SC0012704; FG02-94ER14466; AC02-06CH11357; EAR-0622171
Resource Type:
Accepted Manuscript
Journal Name:
Scientific Reports
Additional Journal Information:
Journal Volume: 5; Journal Issue: 2015; Journal ID: ISSN 2045-2322
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
ENGLISH
Subject:
71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSICS

Citation Formats

Bolmatov, Dima, Zhernenkov, Mikhail, Zav’yalov, Dmitry, Tkachev, Sergey N., Cunsolo, Alessandro, and Cai, Yong Q. The Frenkel Line: a direct experimental evidence for the new thermodynamic boundary. United States: N. p., 2015. Web. doi:10.1038/srep15850.
Bolmatov, Dima, Zhernenkov, Mikhail, Zav’yalov, Dmitry, Tkachev, Sergey N., Cunsolo, Alessandro, & Cai, Yong Q. The Frenkel Line: a direct experimental evidence for the new thermodynamic boundary. United States. doi:10.1038/srep15850.
Bolmatov, Dima, Zhernenkov, Mikhail, Zav’yalov, Dmitry, Tkachev, Sergey N., Cunsolo, Alessandro, and Cai, Yong Q. Thu . "The Frenkel Line: a direct experimental evidence for the new thermodynamic boundary". United States. doi:10.1038/srep15850. https://www.osti.gov/servlets/purl/1235468.
@article{osti_1235468,
title = {The Frenkel Line: a direct experimental evidence for the new thermodynamic boundary},
author = {Bolmatov, Dima and Zhernenkov, Mikhail and Zav’yalov, Dmitry and Tkachev, Sergey N. and Cunsolo, Alessandro and Cai, Yong Q.},
abstractNote = {We report that supercritical fluids play a significant role in elucidating fundamental aspects of liquid matter under extreme conditions. They have been extensively studied at pressures and temperatures relevant to various industrial applications. However, much less is known about the structural behaviour of supercritical fluids and no structural crossovers have been observed in static compression experiments in any temperature and pressure ranges beyond the critical point. The structure of supercritical state is currently perceived to be uniform everywhere on the pressure-temperature phase diagram, and to change only in a monotonic way even moving around the critical point, not only along isotherms or isobars. Conversely, we observe structural crossovers for the first time in a deeply supercritical sample through diffraction measurements in a diamond anvil cell and discover a new thermodynamic boundary on the pressure-temperature diagram. We explain the existence of these crossovers in the framework of the phonon theory of liquids using molecular dynamics simulations. The obtained results are of prime importance since they imply a global reconsideration of the mere essence of the supercritical phase. Furthermore, this discovery may pave the way to new unexpected applications and to the exploration of exotic behaviour of confined fluids relevant to geo- and planetary sciences.},
doi = {10.1038/srep15850},
journal = {Scientific Reports},
number = 2015,
volume = 5,
place = {United States},
year = {2015},
month = {11}
}

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