Multicomponent mutual diffusion in the warm, dense matter regime
Abstract
In this work, we present the formulation, simulations, and results for multicomponent mutual diffusion coefficients in the warm, dense matter regime. While binary mixtures have received considerable attention for mass transport, far fewer studies have addressed ternary and more complex systems. We therefore explicitly examine ternary systems utilizing the Maxwell-Stefan formulation that relates diffusion to gradients in the chemical potential. Onsager coefficients then connect the macroscopic diffusion to microscopic particle motions, evinced in trajectories characterized by positions and velocities, through various autocorrelation functions (ACFs). These trajectories are generated by molecular dynamics (MD) simulations either through the Born-Oppenheimer approximation, which treats the ions classically and the electrons quantum-mechanically by an orbital-free density-functional theory, or through a classical MD approach with Yukawa pair-potentials, whose effective ionizations and electron screening length derive from quantal considerations. We employ the reference-mean form of the ACFs and determine the center-of-mass coefficients through a simple reference-frame-dependent similarity transformation. The Onsager terms in turn determine the mutual diffusion coefficients. We examine a representative sample of ternary mixtures as a function of density and temperature from those with only light elements (D-Li-C, D-Li-Al) to those with highly asymmetric mass components (D-Li-Cu, D-Li-Ag, H-C-Ag). We also follow trends in themore »
- Publication Date:
- Research Org.:
- Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
- Sponsoring Org.:
- USDOE National Nuclear Security Administration (NNSA)
- OSTI Identifier:
- 1856177
- Alternate Identifier(s):
- OSTI ID: 1567881
- Report Number(s):
- LA-UR-22-21786
Journal ID: ISSN 2470-0045; TRN: US2305092
- Grant/Contract Number:
- 89233218CNA000001; 89233218NCA000001
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Physical Review. E
- Additional Journal Information:
- Journal Volume: 100; Journal Issue: 3; Journal ID: ISSN 2470-0045
- Publisher:
- American Physical Society (APS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 70 PLASMA PHYSICS AND FUSION TECHNOLOGY; Plasma transport
Citation Formats
White, A. J., Ticknor, C., Meyer, E. R., Kress, J. D., and Collins, L. A. Multicomponent mutual diffusion in the warm, dense matter regime. United States: N. p., 2019.
Web. doi:10.1103/physreve.100.033213.
White, A. J., Ticknor, C., Meyer, E. R., Kress, J. D., & Collins, L. A. Multicomponent mutual diffusion in the warm, dense matter regime. United States. https://doi.org/10.1103/physreve.100.033213
White, A. J., Ticknor, C., Meyer, E. R., Kress, J. D., and Collins, L. A. Mon .
"Multicomponent mutual diffusion in the warm, dense matter regime". United States. https://doi.org/10.1103/physreve.100.033213. https://www.osti.gov/servlets/purl/1856177.
@article{osti_1856177,
title = {Multicomponent mutual diffusion in the warm, dense matter regime},
author = {White, A. J. and Ticknor, C. and Meyer, E. R. and Kress, J. D. and Collins, L. A.},
abstractNote = {In this work, we present the formulation, simulations, and results for multicomponent mutual diffusion coefficients in the warm, dense matter regime. While binary mixtures have received considerable attention for mass transport, far fewer studies have addressed ternary and more complex systems. We therefore explicitly examine ternary systems utilizing the Maxwell-Stefan formulation that relates diffusion to gradients in the chemical potential. Onsager coefficients then connect the macroscopic diffusion to microscopic particle motions, evinced in trajectories characterized by positions and velocities, through various autocorrelation functions (ACFs). These trajectories are generated by molecular dynamics (MD) simulations either through the Born-Oppenheimer approximation, which treats the ions classically and the electrons quantum-mechanically by an orbital-free density-functional theory, or through a classical MD approach with Yukawa pair-potentials, whose effective ionizations and electron screening length derive from quantal considerations. We employ the reference-mean form of the ACFs and determine the center-of-mass coefficients through a simple reference-frame-dependent similarity transformation. The Onsager terms in turn determine the mutual diffusion coefficients. We examine a representative sample of ternary mixtures as a function of density and temperature from those with only light elements (D-Li-C, D-Li-Al) to those with highly asymmetric mass components (D-Li-Cu, D-Li-Ag, H-C-Ag). We also follow trends in the diffusion as a function of number concentration and evaluated the efficacy of various approximations such as the Darken approximation.},
doi = {10.1103/physreve.100.033213},
journal = {Physical Review. E},
number = 3,
volume = 100,
place = {United States},
year = {Mon Sep 30 00:00:00 EDT 2019},
month = {Mon Sep 30 00:00:00 EDT 2019}
}
Free Publicly Available Full Text
Publisher's Version of Record
Other availability
Search WorldCat to find libraries that may hold this journal
Cited by: 11 works
Citation information provided by
Web of Science
Web of Science
Save to My Library
You must Sign In or Create an Account in order to save documents to your library.
Works referenced in this record:
The role of reference frames in the molecular theory of diffusive transport in solutions
journal, November 1989
- Raineri, Fernando O.; Friedman, Harold L.
- The Journal of Chemical Physics, Vol. 91, Issue 9
High-pressure ionic and molecular phases of ammonia within density functional theory
journal, October 2012
- Griffiths, Gareth I. G.; Needs, R. J.; Pickard, Chris J.
- Physical Review B, Vol. 86, Issue 14
Multicomponent Diffusion.
journal, February 2001
- Curtiss, C. F.; Bird, R. B.
- Industrial & Engineering Chemistry Research, Vol. 40, Issue 7
Material Properties for the Interiors of Massive Giant Planets and Brown Dwarfs
text, January 2018
- Becker, Andreas; Bethkenhagen, Mandy; Kellermann, Clemens
- arXiv
Bonding and structure in dense multi-component molecular mixtures
journal, October 2015
- Meyer, Edmund R.; Ticknor, Christopher; Bethkenhagen, Mandy
- The Journal of Chemical Physics, Vol. 143, Issue 16
Mechanical Basis of Diffusion
journal, November 1962
- Truesdell, C.
- The Journal of Chemical Physics, Vol. 37, Issue 10
Yukawa Monte Carlo and Orbital Free Molecular Dynamics approaches for the equation of state and structural properties of hot dense matter
journal, May 2007
- Gilles, D.; Lambert, F.; Clérouin, J.
- High Energy Density Physics, Vol. 3, Issue 1-2
Fast Parallel Algorithms for Short-Range Molecular Dynamics
journal, March 1995
- Plimpton, Steve
- Journal of Computational Physics, Vol. 117, Issue 1
Superionic Phases of the 1:1 Water–Ammonia Mixture
journal, October 2015
- Bethkenhagen, Mandy; Cebulla, Daniel; Redmer, Ronald
- The Journal of Physical Chemistry A, Vol. 119, Issue 42
Equation of state and phase diagram of ammonia at high pressures from ab initio simulations
journal, June 2013
- Bethkenhagen, Mandy; French, Martin; Redmer, Ronald
- The Journal of Chemical Physics, Vol. 138, Issue 23
Fick Diffusion Coefficients in Ternary Liquid Systems from Equilibrium Molecular Dynamics Simulations
journal, July 2012
- Liu, Xin; Martín-Calvo, Ana; McGarrity, Erin
- Industrial & Engineering Chemistry Research, Vol. 51, Issue 30
Maxwell–Stefan diffusivities in liquid mixtures: Using molecular dynamics for testing model predictions
journal, February 2011
- Liu, Xin; Vlugt, Thijs J. H.; Bardow, André
- Fluid Phase Equilibria, Vol. 301, Issue 1
Predictive Darken Equation for Maxwell-Stefan Diffusivities in Multicomponent Mixtures
journal, September 2011
- Liu, Xin; Vlugt, Thijs J. H.; Bardow, André
- Industrial & Engineering Chemistry Research, Vol. 50, Issue 17
Planetary Ices and the Linear Mixing Approximation
journal, October 2017
- Bethkenhagen, M.; Meyer, E. R.; Hamel, S.
- The Astrophysical Journal, Vol. 848, Issue 1
Effect of correlation on viscosity and diffusion in molecular-dynamics simulations
journal, October 2014
- Meyer, Edmund R.; Kress, Joel D.; Collins, Lee A.
- Physical Review E, Vol. 90, Issue 4
Transport properties of lithium hydride at extreme conditions from orbital-free molecular dynamics
journal, February 2013
- Burakovsky, L.; Ticknor, C.; Kress, J. D.
- Physical Review E, Vol. 87, Issue 2
Diffusion in multicomponent liquids: A new set of collective velocity correlation functions and diffusion coefficients
journal, September 1993
- Trullàs, J.; Padró, J. A.
- The Journal of Chemical Physics, Vol. 99, Issue 5
Viscosity and mutual diffusion in strongly asymmetric binary ionic mixtures
text, January 2006
- Bastea, Sorin
- arXiv
A Review of Equation-of-State Models for Inertial Confinement Fusion Materials
journal, September 2018
- Gaffney, J. A.; Hu, S. X.; Arnault, P.
- High Energy Density Physics, Vol. 28
The Darken Relation for Multicomponent Diffusion in Liquid Mixtures of Linear Alkanes: An Investigation Using Molecular Dynamics (MD) Simulations
journal, August 2005
- Krishna, R.; van Baten, J. M.
- Industrial & Engineering Chemistry Research, Vol. 44, Issue 17
Molecular dynamics evaluation of self-diffusion in Yukawa systems
journal, November 2000
- Ohta, H.; Hamaguchi, S.
- Physics of Plasmas, Vol. 7, Issue 11
Observation of Ultrafast Solid-Density Plasma Dynamics Using Femtosecond X-Ray Pulses from a Free-Electron Laser
journal, September 2018
- Kluge, Thomas; Rödel, Melanie; Metzkes-Ng, Josefine
- Physical Review X, Vol. 8, Issue 3
Phase Diagram and Electrical Conductivity of High Energy-Density Water from Density Functional Theory
journal, July 2006
- Mattsson, Thomas R.; Desjarlais, Michael P.
- Physical Review Letters, Vol. 97, Issue 1
Green−Kubo Formulas for Mutual Diffusion Coefficients in Multicomponent Systems
journal, January 1996
- Zhou, Yanhua; Miller, Gregory H.
- The Journal of Physical Chemistry, Vol. 100, Issue 13
Diffusion Coefficients from Molecular Dynamics Simulations in Binary and Ternary Mixtures
journal, July 2013
- Liu, Xin; Schnell, Sondre K.; Simon, Jean-Marc
- International Journal of Thermophysics, Vol. 34, Issue 7
Kirkwood–Buff Integrals for Finite Volumes
journal, December 2012
- Krüger, Peter; Schnell, Sondre K.; Bedeaux, Dick
- The Journal of Physical Chemistry Letters, Vol. 4, Issue 2
Material Properties for the Interiors of Massive Giant Planets and Brown Dwarfs
journal, September 2018
- Becker, Andreas; Bethkenhagen, Mandy; Kellermann, Clemens
- The Astronomical Journal, Vol. 156, Issue 4
Viscosity and mutual diffusion of deuterium-tritium mixtures in the warm-dense-matter regime
journal, September 2010
- Kress, J. D.; Cohen, James S.; Horner, D. A.
- Physical Review E, Vol. 82, Issue 3
Inversion of multicomponent diffusion equations
journal, August 2005
- Matuszak, Daniel; Donohue, Marc D.
- Chemical Engineering Science, Vol. 60, Issue 15
Gradient correction to the statistical electronic free energy at nonzero temperatures: Application to equation-of-state calculations
journal, August 1979
- Perrot, F.
- Physical Review A, Vol. 20, Issue 2
A calculation method for multicomponent mass transfer coefficient correlations
journal, November 1999
- Alopaeus, Ville; Nordén, Harry V.
- Computers & Chemical Engineering, Vol. 23, Issue 9
Diffusivity in asymmetric Yukawa ionic mixtures in dense plasmas
journal, August 2014
- Haxhimali, Tomorr; Rudd, Robert E.; Cabot, William H.
- Physical Review E, Vol. 90, Issue 2
The mutual diffusion coefficient D 12 in binary liquid model mixtures. Molecular dynamics calculations based on Lennard-Jones (12-6) potentials : I. The method of determination
journal, May 1984
- Schoen, M.; Hoheisel, C.
- Molecular Physics, Vol. 52, Issue 1
Time-dependent orbital-free density functional theory for electronic stopping power: Comparison to the Mermin-Kohn-Sham theory at high temperatures
journal, October 2018
- White, Alexander J.; Certik, Ondrej; Ding, Y. H.
- Physical Review B, Vol. 98, Issue 14
Transport properties of an asymmetric mixture in the dense plasma regime
journal, June 2016
- Ticknor, Christopher; Kress, Joel D.; Collins, Lee A.
- Physical Review E, Vol. 93, Issue 6
Observation of ultrafast solid-density plasma dynamics using femtosecond X-ray pulses from a free-electron laser
text, January 2018
- Kluge, Thomas; Rödel, Melanie; Metzkes, Josefine
- arXiv
Benchmarking the diffusion and viscosity of H-He mixtures in warm dense matter regime by quantum molecular dynamics simulations
journal, May 2017
- Li, Zhi-Guo; Zhang, Wei; Fu, Zhi-Jian
- Physics of Plasmas, Vol. 24, Issue 5
Experimental validation of thermodynamic mixture rules at extreme pressures and densities
journal, January 2018
- Bradley, P. A.; Loomis, E. N.; Merritt, E. C.
- Physics of Plasmas, Vol. 25, Issue 1
Correlation and transport properties for mixtures at constant pressure and temperature
journal, June 2017
- White, Alexander J.; Collins, Lee A.; Kress, Joel D.
- Physical Review E, Vol. 95, Issue 6
Experimental evidence for superionic water ice using shock compression
journal, February 2018
- Millot, Marius; Hamel, Sebastien; Rygg, J. Ryan
- Nature Physics, Vol. 14, Issue 3
A review on ab initio studies of static, transport, and optical properties of polystyrene under extreme conditions for inertial confinement fusion applications
journal, May 2018
- Collins, L. A.; Boehly, T. R.; Ding, Y. H.
- Physics of Plasmas, Vol. 25, Issue 5
Equation of state of dense plasmas by ab initio simulations: Bridging the gap between quantum molecular dynamics and orbital-free molecular dynamics at high temperature
journal, December 2012
- Danel, J. -F.; Kazandjian, L.; Zérah, G.
- Physics of Plasmas, Vol. 19, Issue 12
Ab initio molecular dynamics with an orbital-free density functional
journal, May 1993
- Pearson, M.; Smargiassi, E.; Madden, P. A.
- Journal of Physics: Condensed Matter, Vol. 5, Issue 19
Combining Kohn-Sham and orbital-free density-functional theory for Hugoniot calculations to extreme pressures
journal, December 2014
- Sheppard, Daniel; Kress, Joel D.; Crockett, Scott
- Physical Review E, Vol. 90, Issue 6
Multicomponent Diffusion
journal, July 1999
- Curtiss, C. F.; Bird, R. Byron
- Industrial & Engineering Chemistry Research, Vol. 38, Issue 7
Fick Diffusion Coefficients of Liquid Mixtures Directly Obtained From Equilibrium Molecular Dynamics
journal, November 2011
- Liu, Xin; Schnell, Sondre K.; Simon, Jean-Marc
- The Journal of Physical Chemistry B, Vol. 115, Issue 44
Molecular Dynamics Simulations of Multicomponent Diffusion. 1. Equilibrium Method
journal, November 2004
- Wheeler, Dean R.; Newman, John
- The Journal of Physical Chemistry B, Vol. 108, Issue 47
The Maxwell-Stefan approach to mass transfer
journal, March 1997
- Krishna, R.; Wesselingh, J. A.
- Chemical Engineering Science, Vol. 52, Issue 6
Self-interaction correction to density-functional approximations for many-electron systems
journal, May 1981
- Perdew, J. P.; Zunger, Alex
- Physical Review B, Vol. 23, Issue 10, p. 5048-5079
Viscosity and mutual diffusion in strongly asymmetric binary ionic mixtures
journal, May 2005
- Bastea, Sorin
- Physical Review E, Vol. 71, Issue 5
Form of multicomponent Fickian diffusion coefficients matrix
journal, August 2011
- Wambui Mutoru, J.; Firoozabadi, Abbas
- The Journal of Chemical Thermodynamics, Vol. 43, Issue 8
Unified description of linear screening in dense plasmas
journal, March 2015
- Stanton, L. G.; Murillo, M. S.
- Physical Review E, Vol. 91, Issue 3
Multicomponent Maxwell−Stefan Diffusivities at Infinite Dilution
journal, April 2011
- Liu, Xin; Bardow, André; Vlugt, Thijs J. H.
- Industrial & Engineering Chemistry Research, Vol. 50, Issue 8
Finite-size effects of Kirkwood–Buff integrals from molecular simulations
journal, December 2017
- Dawass, N.; Krüger, P.; Schnell, S. K.
- Molecular Simulation, Vol. 44, Issue 7
Ab Initio Studies on the Stopping Power of Warm Dense Matter with Time-Dependent Orbital-Free Density Functional Theory
journal, October 2018
- Ding, Y. H.; White, A. J.; Hu, S. X.
- Physical Review Letters, Vol. 121, Issue 14
Diffusion Coefficients of a Highly Nonideal Ternary Liquid Mixture: Cyclohexane–Toluene–Methanol
journal, October 2018
- Janzen, Tatjana; Vrabec, Jadran
- Industrial & Engineering Chemistry Research, Vol. 57, Issue 48