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Title: Revealing the mechanism of the viscous-to-elastic crossover in liquids

Abstract

In our work, we report on inelastic X-ray scattering experiments combined with the molecular dynamics simulations on deeply supercritical Ar. Our results unveil the mechanism and regimes of sound propagation in the liquid matter and provide compelling evidence for the adiabatic-to-isothermal longitudinal sound propagation transition. We introduce a Hamiltonian predicting low-frequency transverse sound propagation gaps, which is confirmed by experimental findings and molecular dynamics calculations. As a result, a universal link is established between the positive sound dispersion (PSD) phenomenon and the origin of transverse sound propagation revealing the viscous-to-elastic crossover in liquids. The PSD and transverse phononic excitations evolve consistently with theoretical predictions. Both can be considered as a universal fingerprint of the dynamic response of a liquid, which is also observable in a subdomain of supercritical phase. Furthermore, the simultaneous disappearance of both these effects at elevated temperatures is a manifestation of the Frenkel line. We expect that these findings will advance the current understanding of fluids under extreme thermodynamic conditions.

Authors:
 [1];  [1];  [2];  [3];  [1];  [1]
  1. Brookhaven National Lab. (BNL), Upton, NY (United States)
  2. Volgograd State Technical Univ. (Russia)
  3. Argonne National Lab. (ANL), Argonne, IL (United States)
Publication Date:
Research Org.:
Brookhaven National Laboratory (BNL), Upton, NY (United States)
Sponsoring Org.:
USDOE Office of Science (SC)
OSTI Identifier:
1237164
Report Number(s):
BNL-108218-2015-JA
Journal ID: ISSN 1948-7185; R&D Project: LS001
Grant/Contract Number:  
SC00112704
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Journal of Physical Chemistry Letters
Additional Journal Information:
Journal Volume: 6; Journal Issue: 15; Journal ID: ISSN 1948-7185
Publisher:
American Chemical Society
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE

Citation Formats

Bolmatov, Dima, Zhernenkov, Mikhail, Zav'yalov, Dmitry, Stoupin, Stanislav, Cai, Yong Q., and Cunsolo, Alessandro. Revealing the mechanism of the viscous-to-elastic crossover in liquids. United States: N. p., 2015. Web. doi:10.1021/acs.jpclett.5b01338.
Bolmatov, Dima, Zhernenkov, Mikhail, Zav'yalov, Dmitry, Stoupin, Stanislav, Cai, Yong Q., & Cunsolo, Alessandro. Revealing the mechanism of the viscous-to-elastic crossover in liquids. United States. https://doi.org/10.1021/acs.jpclett.5b01338
Bolmatov, Dima, Zhernenkov, Mikhail, Zav'yalov, Dmitry, Stoupin, Stanislav, Cai, Yong Q., and Cunsolo, Alessandro. 2015. "Revealing the mechanism of the viscous-to-elastic crossover in liquids". United States. https://doi.org/10.1021/acs.jpclett.5b01338. https://www.osti.gov/servlets/purl/1237164.
@article{osti_1237164,
title = {Revealing the mechanism of the viscous-to-elastic crossover in liquids},
author = {Bolmatov, Dima and Zhernenkov, Mikhail and Zav'yalov, Dmitry and Stoupin, Stanislav and Cai, Yong Q. and Cunsolo, Alessandro},
abstractNote = {In our work, we report on inelastic X-ray scattering experiments combined with the molecular dynamics simulations on deeply supercritical Ar. Our results unveil the mechanism and regimes of sound propagation in the liquid matter and provide compelling evidence for the adiabatic-to-isothermal longitudinal sound propagation transition. We introduce a Hamiltonian predicting low-frequency transverse sound propagation gaps, which is confirmed by experimental findings and molecular dynamics calculations. As a result, a universal link is established between the positive sound dispersion (PSD) phenomenon and the origin of transverse sound propagation revealing the viscous-to-elastic crossover in liquids. The PSD and transverse phononic excitations evolve consistently with theoretical predictions. Both can be considered as a universal fingerprint of the dynamic response of a liquid, which is also observable in a subdomain of supercritical phase. Furthermore, the simultaneous disappearance of both these effects at elevated temperatures is a manifestation of the Frenkel line. We expect that these findings will advance the current understanding of fluids under extreme thermodynamic conditions.},
doi = {10.1021/acs.jpclett.5b01338},
url = {https://www.osti.gov/biblio/1237164}, journal = {Journal of Physical Chemistry Letters},
issn = {1948-7185},
number = 15,
volume = 6,
place = {United States},
year = {Sat Jul 18 00:00:00 EDT 2015},
month = {Sat Jul 18 00:00:00 EDT 2015}
}

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Cited by: 40 works
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Works referenced in this record:

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journal, June 2010


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journal, September 2013


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journal, December 2013


Temperature-induced ruby fluorescence shifts up to a pressure of 15 GPa in an externally heated diamond anvil cell
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Thermodynamic behavior of supercritical matter
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