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 »
- Authors:
-
- Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
- 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}
}
Web of Science
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