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:
-
- Brookhaven National Lab. (BNL), Upton, NY (United States)
- Volgograd State Technical Univ. (Russia)
- 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}
}
Web of Science
Works referenced in this record:
Microscopic relaxation in supercritical and liquid neon
journal, February 2001
- Cunsolo, A.; Pratesi, G.; Verbeni, R.
- The Journal of Chemical Physics, Vol. 114, Issue 5
Structural and Collisional Relaxations in Liquids and Supercritical Fluids
journal, February 2007
- Bencivenga, F.; Cunsolo, A.; Krisch, M.
- Physical Review Letters, Vol. 98, Issue 8
The Widom line as the crossover between liquid-like and gas-like behaviour in supercritical fluids
journal, June 2010
- Simeoni, G. G.; Bryk, T.; Gorelli, F. A.
- Nature Physics, Vol. 6, Issue 7
Symmetry breaking gives rise to energy spectra of three states of matter
journal, September 2013
- Bolmatov, Dima; Musaev, Edvard T.; Trachenko, K.
- Scientific Reports, Vol. 3, Issue 1
Thermodynamic behaviour of supercritical matter
journal, August 2013
- Bolmatov, Dima; Brazhkin, V. V.; Trachenko, K.
- Nature Communications, Vol. 4, Issue 1
Evidence for structural crossover in the supercritical state
journal, December 2013
- Bolmatov, Dima; Brazhkin, V. V.; Fomin, Yu. D.
- The Journal of Chemical Physics, Vol. 139, Issue 23
Structural Evolution of Supercritical CO 2 across the Frenkel Line
journal, August 2014
- Bolmatov, Dima; Zav’yalov, D.; Gao, M.
- The Journal of Physical Chemistry Letters, Vol. 5, Issue 16
Short-Wavelength Sound Modes in Liquid Argon
journal, March 1983
- de Schepper, I. M.; Verkerk, P.; van Well, A. A.
- Physical Review Letters, Vol. 50, Issue 13
Liquid argon: Monte carlo and molecular dynamics calculations
journal, January 1971
- Barker, J. A.; Fisher, R. A.; Watts, R. O.
- Molecular Physics, Vol. 21, Issue 4
Microscopic sound waves in dense Lennard-Jones fluids
journal, March 1984
- de Schepper, I. M.; van Rijs, J. C.; van Well, A. A.
- Physical Review A, Vol. 29, Issue 3
Water Phase Diagram Is Significantly Altered by Imidazolium Ionic Liquid
journal, April 2014
- Chaban, Vitaly V.; Prezhdo, Oleg V.
- The Journal of Physical Chemistry Letters, Vol. 5, Issue 10
Vapor–Liquid Coexistence and Critical Behavior of Ionic Liquids via Molecular Simulations
journal, May 2011
- Rai, Neeraj; Maginn, Edward J.
- The Journal of Physical Chemistry Letters, Vol. 2, Issue 12
Liquid–Liquid Phase Transition and Its Phase Diagram in Deeply-Cooled Heavy Water Confined in a Nanoporous Silica Matrix
journal, May 2015
- Wang, Zhe; Ito, Kanae; Leão, Juscelino B.
- The Journal of Physical Chemistry Letters, Vol. 6, Issue 11
Liquid-Phase Vibrational Strong Coupling
journal, March 2015
- George, Jino; Shalabney, Atef; Hutchison, James A.
- The Journal of Physical Chemistry Letters, Vol. 6, Issue 6
The phonon theory of liquid thermodynamics
journal, May 2012
- Bolmatov, D.; Brazhkin, V. V.; Trachenko, K.
- Scientific Reports, Vol. 2, Issue 1
Liquid heat capacity in the approach from the solid state: Anharmonic theory
journal, August 2011
- Bolmatov, Dima; Trachenko, Kostya
- Physical Review B, Vol. 84, Issue 5
Specific Heat Anomaly in a Supercooled Liquid with Amorphous Boundary Conditions
journal, June 2015
- Mártin, Daniel A.; Cavagna, Andrea; Grigera, Tomás S.
- Physical Review Letters, Vol. 114, Issue 22
BX90: A new diamond anvil cell design for X-ray diffraction and optical measurements
journal, December 2012
- Kantor, I.; Prakapenka, V.; Kantor, A.
- Review of Scientific Instruments, Vol. 83, Issue 12, Article No. 125102
The COMPRES/GSECARS gas-loading system for diamond anvil cells at the Advanced Photon Source
journal, September 2008
- Rivers, Mark; Prakapenka, Vitali; Kubo, Atsushi
- High Pressure Research, Vol. 28, Issue 3
Temperature-induced ruby fluorescence shifts up to a pressure of 15 GPa in an externally heated diamond anvil cell
journal, January 1999
- Rekhi, Sandeep; Dubrovinsky, Leonid; Saxena, Surendra
- High Temperatures-High Pressures, Vol. 31, Issue 3
Quantum effects in the dynamics of He probed by inelastic x-ray scattering
journal, July 2001
- Verbeni, R.; Cunsolo, A.; Pratesi, G.
- Physical Review E, Vol. 64, Issue 2
Signatures of quantum behavior in the microscopic dynamics of liquid hydrogen and deuterium
journal, September 2005
- Cunsolo, A.; Colognesi, D.; Sampoli, M.
- The Journal of Chemical Physics, Vol. 123, Issue 11
Adiabatic and isothermal sound waves: The case of supercritical nitrogen
journal, July 2006
- Bencivenga, F.; Cunsolo, A.; Krisch, M.
- Europhysics Letters (EPL), Vol. 75, Issue 1
Mixing of Longitudinal and Transverse Dynamics in Liquid Water
journal, September 1997
- Sampoli, M.; Ruocco, G.; Sette, F.
- Physical Review Letters, Vol. 79, Issue 9
The Widom line as the crossover between liquid-like and gas-like behaviour in supercritical fluids
journal, June 2010
- Simeoni, G. G.; Bryk, T.; Gorelli, F. A.
- Nature Physics, Vol. 6, Issue 7
The phonon theory of liquid thermodynamics
journal, May 2012
- Bolmatov, D.; Brazhkin, V. V.; Trachenko, K.
- Scientific Reports, Vol. 2, Issue 1
Symmetry breaking gives rise to energy spectra of three states of matter
journal, September 2013
- Bolmatov, Dima; Musaev, Edvard T.; Trachenko, K.
- Scientific Reports, Vol. 3, Issue 1
Evidence for structural crossover in the supercritical state
journal, December 2013
- Bolmatov, Dima; Brazhkin, V. V.; Fomin, Yu. D.
- The Journal of Chemical Physics, Vol. 139, Issue 23
Temperature-induced ruby fluorescence shifts up to a pressure of 15 GPa in an externally heated diamond anvil cell
journal, January 1999
- Rekhi, Sandeep; Dubrovinsky, Leonid; Saxena, Surendra
- High Temperatures-High Pressures, Vol. 31, Issue 3
Liquidlike Behavior of Supercritical Fluids
journal, December 2006
- Gorelli, F.; Santoro, M.; Scopigno, T.
- Physical Review Letters, Vol. 97, Issue 24
Liquid heat capacity in the approach from the solid state: anharmonic theory
text, January 2011
- Bolmatov, Dima; Trachenko, Kostya
- arXiv
Thermodynamic behavior of supercritical matter
text, January 2013
- Bolmatov, Dima; Brazhkin, V. V.; Trachenko, K.
- arXiv
Adiabatic and isothermal sound waves: the case of supercritical nitrogen
text, January 2005
- Bencivenga, F.; Cunsolo, A.; Krisch, M.
- arXiv
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Instantaneous shear modulus of Yukawa fluids across coupling regimes
journal, February 2020
- Khrapak, Sergey A.; Klumov, Boris A.
- Physics of Plasmas, Vol. 27, Issue 2
Continuum mechanics with torsion
journal, April 2019
- Peshkov, Ilya; Romenski, Evgeniy; Dumbser, Michael
- Continuum Mechanics and Thermodynamics, Vol. 31, Issue 5
Revealing the mechanism of passive transport in lipid bilayers via phonon-mediated nanometre-scale density fluctuations
journal, May 2016
- Zhernenkov, Mikhail; Bolmatov, Dima; Soloviov, Dmitry
- Nature Communications, Vol. 7, Issue 1
Continuum mechanics and thermodynamics in the Hamilton and the Godunov-type formulations
journal, January 2018
- Peshkov, Ilya; Pavelka, Michal; Romenski, Evgeniy
- Continuum Mechanics and Thermodynamics, Vol. 30, Issue 6
Mechanical heterogeneity in ionic liquids
journal, May 2018
- Veldhorst, Arno A.; Ribeiro, Mauro C. C.
- The Journal of Chemical Physics, Vol. 148, Issue 19
A Unified Hyperbolic Formulation for Viscous Fluids and Elastoplastic Solids
book, January 2018
- Dumbser, Michael; Peshkov, Ilya; Romenski, Evgeniy
- Theory, Numerics and Applications of Hyperbolic Problems II
Onset of transverse (shear) waves in strongly-coupled Yukawa fluids
journal, March 2019
- Khrapak, Sergey A.; Khrapak, Alexey G.; Kryuchkov, Nikita P.
- The Journal of Chemical Physics, Vol. 150, Issue 10
Thermally triggered phononic gaps in liquids at THz scale
journal, January 2016
- Bolmatov, Dima; Zhernenkov, Mikhail; Zav’yalov, Dmitry
- Scientific Reports, Vol. 6, Issue 1
Continuum mechanics with torsion
text, January 2018
- Peshkov, Ilya; Romenski, Evgeniy; Dumbser, Michael
- arXiv
Instantaneous shear modulus of Yukawa fluids across coupling regimes
text, January 2020
- Khrapak, Sergey; Klumov, Boris
- arXiv
High order ADER schemes for a unified first order hyperbolic formulation of continuum mechanics: Viscous heat-conducting fluids and elastic solids
journal, June 2016
- Dumbser, Michael; Peshkov, Ilya; Romenski, Evgeniy
- Journal of Computational Physics, Vol. 314
Revealing the mechanism of passive transport in lipid bilayers via phonon-mediated nanometre-scale density fluctuations
journal, May 2016
- Zhernenkov, Mikhail; Bolmatov, Dima; Soloviov, Dmitry
- Nature Communications, Vol. 7, Issue 1
Functional lipid pairs as building blocks of phase-separated membranes
journal, February 2020
- Soloviov, Dmytro; Cai, Yong Q.; Bolmatov, Dima
- Proceedings of the National Academy of Sciences, Vol. 117, Issue 9
A unified hyperbolic formulation for viscous fluids and elastoplastic solids
text, January 2017
- Peshkov, Ilya; Romenski, Evgeniy; Dumbser, Michael
- arXiv