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Title: Fluctuating hydrodynamics of reactive liquid mixtures

Abstract

Fluctuating hydrodynamics (FHD) provides a framework for modeling microscopic fluctuations in a manner consistent with statistical mechanics and nonequilibrium thermodynamics. This paper presents an FHD formulation for isothermal reactive incompressible liquid mixtures with stochastic chemistry. Fluctuating multispecies mass diffusion is formulated using a Maxwell-Stefan description without assuming a dilute solution, and momentum dynamics is described by a stochastic Navier-Stokes equation for the fluid velocity. We consider a thermodynamically consistent generalization for the law of mass action for non-dilute mixtures and use it in the chemical master equation (CME) to model reactions as a Poisson process. The FHD approach provides remarkable computational efficiency over traditional reaction-diffusion master equation methods when the number of reactive molecules is large, while also retaining accuracy even when there are as few as ten reactive molecules per hydrodynamic cell. We present a numerical algorithm to solve the coupled FHD and CME equations and validate it on both equilibrium and nonequilibrium problems. We simulate a diffusively driven gravitational instability in the presence of an acid-base neutralization reaction, starting from a perfectly flat interface. We demonstrate that the coupling between velocity and concentration fluctuations dominates the initial growth of the instability.

Authors:
 [1];  [2];  [2];  [3];  [4]
  1. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Computational Research Div.; Univ. of California, Merced, CA (United States). Applied Mathematics
  2. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Computational Research Div.
  3. San Jose State Univ., San Jose, CA (United States). Dept. of Physics and Astronomy
  4. New York Univ. (NYU), NY (United States). Courant Institute of Mathematical Sciences
Publication Date:
Research Org.:
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Advanced Scientific Computing Research (ASCR) (SC-21)
OSTI Identifier:
1526536
Alternate Identifier(s):
OSTI ID: 1467940
Grant/Contract Number:  
[AC02-05CH11231; SC0008271]
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Chemical Physics
Additional Journal Information:
[ Journal Volume: 149; Journal Issue: 8]; Journal ID: ISSN 0021-9606
Publisher:
American Institute of Physics (AIP)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Kim, Changho, Nonaka, Andy, Bell, John B., Garcia, Alejandro L., and Donev, Aleksandar. Fluctuating hydrodynamics of reactive liquid mixtures. United States: N. p., 2018. Web. doi:10.1063/1.5043428.
Kim, Changho, Nonaka, Andy, Bell, John B., Garcia, Alejandro L., & Donev, Aleksandar. Fluctuating hydrodynamics of reactive liquid mixtures. United States. doi:10.1063/1.5043428.
Kim, Changho, Nonaka, Andy, Bell, John B., Garcia, Alejandro L., and Donev, Aleksandar. Tue . "Fluctuating hydrodynamics of reactive liquid mixtures". United States. doi:10.1063/1.5043428. https://www.osti.gov/servlets/purl/1526536.
@article{osti_1526536,
title = {Fluctuating hydrodynamics of reactive liquid mixtures},
author = {Kim, Changho and Nonaka, Andy and Bell, John B. and Garcia, Alejandro L. and Donev, Aleksandar},
abstractNote = {Fluctuating hydrodynamics (FHD) provides a framework for modeling microscopic fluctuations in a manner consistent with statistical mechanics and nonequilibrium thermodynamics. This paper presents an FHD formulation for isothermal reactive incompressible liquid mixtures with stochastic chemistry. Fluctuating multispecies mass diffusion is formulated using a Maxwell-Stefan description without assuming a dilute solution, and momentum dynamics is described by a stochastic Navier-Stokes equation for the fluid velocity. We consider a thermodynamically consistent generalization for the law of mass action for non-dilute mixtures and use it in the chemical master equation (CME) to model reactions as a Poisson process. The FHD approach provides remarkable computational efficiency over traditional reaction-diffusion master equation methods when the number of reactive molecules is large, while also retaining accuracy even when there are as few as ten reactive molecules per hydrodynamic cell. We present a numerical algorithm to solve the coupled FHD and CME equations and validate it on both equilibrium and nonequilibrium problems. We simulate a diffusively driven gravitational instability in the presence of an acid-base neutralization reaction, starting from a perfectly flat interface. We demonstrate that the coupling between velocity and concentration fluctuations dominates the initial growth of the instability.},
doi = {10.1063/1.5043428},
journal = {Journal of Chemical Physics},
number = [8],
volume = [149],
place = {United States},
year = {2018},
month = {8}
}

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