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Title: Applying molecular theory to steady-state diffusing systems

Abstract

Predicting the properties of nonequilibrium systems from molecular simulations is a growing area of interest. One important class of problems involves steady-state diffusion. To study these cases, a grand canonical molecular dynamics approach has been developed by Heffelfinger and van Swol [J. Chem. Phys. 101, 5274 (1994)]. With this method, the flux of particles, the chemical potential gradients, and density gradients can all be measured in the simulation. In this paper, we present a complementary approach that couples a nonlocal density functional theory (DFT) with a transport equation describing steady-state flux of the particles. We compare transport-DFT predictions to GCMD results for a variety of ideal (color diffusion), and nonideal (uphill diffusion and convective transport) systems. In all cases, excellent agreement between transport-DFT and GCMD calculations is obtained with diffusion coefficients that are invariant with respect to density and external fields. (c) 2000 American Institute of Physics.

Authors:
 [1];  [1];  [2]
  1. Department of Computational Biology and Materials Technology, Sandia National Laboratories, Albuquerque, New Mexico 87185 (United States)
  2. Department of Parallel Computational Sciences, Sandia National Laboratories, Albuquerque, New Mexico 87185 (United States)
Publication Date:
OSTI Identifier:
20216010
Resource Type:
Journal Article
Journal Name:
Journal of Chemical Physics
Additional Journal Information:
Journal Volume: 112; Journal Issue: 17; Other Information: PBD: 1 May 2000; Journal ID: ISSN 0021-9606
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL AND ANALYTICAL CHEMISTRY; DIFFUSION; TRANSPORT THEORY; MOLECULES; DENSITY; THEORETICAL DATA

Citation Formats

Frink, Laura J. Douglas, Thompson, Aidan, and Salinger, Andrew G. Applying molecular theory to steady-state diffusing systems. United States: N. p., 2000. Web. doi:10.1063/1.481376.
Frink, Laura J. Douglas, Thompson, Aidan, & Salinger, Andrew G. Applying molecular theory to steady-state diffusing systems. United States. doi:10.1063/1.481376.
Frink, Laura J. Douglas, Thompson, Aidan, and Salinger, Andrew G. Mon . "Applying molecular theory to steady-state diffusing systems". United States. doi:10.1063/1.481376.
@article{osti_20216010,
title = {Applying molecular theory to steady-state diffusing systems},
author = {Frink, Laura J. Douglas and Thompson, Aidan and Salinger, Andrew G.},
abstractNote = {Predicting the properties of nonequilibrium systems from molecular simulations is a growing area of interest. One important class of problems involves steady-state diffusion. To study these cases, a grand canonical molecular dynamics approach has been developed by Heffelfinger and van Swol [J. Chem. Phys. 101, 5274 (1994)]. With this method, the flux of particles, the chemical potential gradients, and density gradients can all be measured in the simulation. In this paper, we present a complementary approach that couples a nonlocal density functional theory (DFT) with a transport equation describing steady-state flux of the particles. We compare transport-DFT predictions to GCMD results for a variety of ideal (color diffusion), and nonideal (uphill diffusion and convective transport) systems. In all cases, excellent agreement between transport-DFT and GCMD calculations is obtained with diffusion coefficients that are invariant with respect to density and external fields. (c) 2000 American Institute of Physics.},
doi = {10.1063/1.481376},
journal = {Journal of Chemical Physics},
issn = {0021-9606},
number = 17,
volume = 112,
place = {United States},
year = {2000},
month = {5}
}