Bonding and structure in dense multi-component molecular mixtures
Abstract
We have performed finite-temperature density functional theory molecular dynamics simulations on dense methane, ammonia, and water mixtures (CH4:NH3:H2O) for various compositions and temperatures (2000 K ≤ T ≤ 10000 K) that span a set of possible conditions in the interiors of ice-giant exoplanets. The equation-of-state, pair distribution functions, and bond autocorrelation functions (BACF) were used to probe the structure and dynamics of these complex fluids. In particular, an improvement to the choice of the cutoff in the BACF was developed that allowed analysis refinements for density and temperature effects. We note the relative changes in the nature of these systems engendered by variations in the concentration ratios. As a result, a basic tenet emerges from all these comparisons that varying the relative amounts of the three heavy components (C,N,O) can effect considerable changes in the nature of the fluid and may in turn have ramifications for the structure and composition of various planetary layers.
- Authors:
-
- Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
- Univ. Rostock, Rostock (Germany)
- Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States)
- Publication Date:
- Research Org.:
- Los Alamos National Laboratory (LANL), Los Alamos, NM (United States)
- Sponsoring Org.:
- USDOE
- OSTI Identifier:
- 1236706
- Alternate Identifier(s):
- OSTI ID: 1224734
- Report Number(s):
- LA-UR-15-22061
Journal ID: ISSN 0021-9606; JCPSA6
- Grant/Contract Number:
- SFB 652; AC52-06NA25396
- Resource Type:
- Journal Article: Accepted Manuscript
- Journal Name:
- Journal of Chemical Physics
- Additional Journal Information:
- Journal Volume: 143; Journal Issue: 16; Journal ID: ISSN 0021-9606
- Publisher:
- American Institute of Physics (AIP)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 79 ASTRONOMY AND ASTROPHYSICS; 75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY; carbon; methane; molecular dynamics; complex fluids; bond formation
Citation Formats
Meyer, Edmund R., Ticknor, Christopher, Bethkenhagen, Mandy, Hamel, Sebastien, Redmer, Ronald, Kress, Joel D., and Collins, Lee A. Bonding and structure in dense multi-component molecular mixtures. United States: N. p., 2015.
Web. doi:10.1063/1.4934626.
Meyer, Edmund R., Ticknor, Christopher, Bethkenhagen, Mandy, Hamel, Sebastien, Redmer, Ronald, Kress, Joel D., & Collins, Lee A. Bonding and structure in dense multi-component molecular mixtures. United States. https://doi.org/10.1063/1.4934626
Meyer, Edmund R., Ticknor, Christopher, Bethkenhagen, Mandy, Hamel, Sebastien, Redmer, Ronald, Kress, Joel D., and Collins, Lee A. 2015.
"Bonding and structure in dense multi-component molecular mixtures". United States. https://doi.org/10.1063/1.4934626. https://www.osti.gov/servlets/purl/1236706.
@article{osti_1236706,
title = {Bonding and structure in dense multi-component molecular mixtures},
author = {Meyer, Edmund R. and Ticknor, Christopher and Bethkenhagen, Mandy and Hamel, Sebastien and Redmer, Ronald and Kress, Joel D. and Collins, Lee A.},
abstractNote = {We have performed finite-temperature density functional theory molecular dynamics simulations on dense methane, ammonia, and water mixtures (CH4:NH3:H2O) for various compositions and temperatures (2000 K ≤ T ≤ 10000 K) that span a set of possible conditions in the interiors of ice-giant exoplanets. The equation-of-state, pair distribution functions, and bond autocorrelation functions (BACF) were used to probe the structure and dynamics of these complex fluids. In particular, an improvement to the choice of the cutoff in the BACF was developed that allowed analysis refinements for density and temperature effects. We note the relative changes in the nature of these systems engendered by variations in the concentration ratios. As a result, a basic tenet emerges from all these comparisons that varying the relative amounts of the three heavy components (C,N,O) can effect considerable changes in the nature of the fluid and may in turn have ramifications for the structure and composition of various planetary layers.},
doi = {10.1063/1.4934626},
url = {https://www.osti.gov/biblio/1236706},
journal = {Journal of Chemical Physics},
issn = {0021-9606},
number = 16,
volume = 143,
place = {United States},
year = {Fri Oct 30 00:00:00 EDT 2015},
month = {Fri Oct 30 00:00:00 EDT 2015}
}
Web of Science
Works referenced in this record:
Symmetric Inertial Confinement Fusion Implosions at Ultra-High Laser Energies
journal, January 2010
- Glenzer, S. H.; MacGowan, B. J.; Michel, P.
- Science, Vol. 327, Issue 5970
Atomic mix in directly driven inertial confinement implosions
journal, November 2011
- Wilson, D. C.; Ebey, P. S.; Sangster, T. C.
- Physics of Plasmas, Vol. 18, Issue 11
Interaction of Nanoparticles with Ideal Liquid-Liquid Interfaces
journal, February 2009
- Cheung, David L.; Bon, Stefan A. F.
- Physical Review Letters, Vol. 102, Issue 6
Interior Structure of Neptune: Comparison with Uranus
journal, August 1991
- Hubbard, W. B.; Nellis, W. J.; Mitchell, A. C.
- Science, Vol. 253, Issue 5020
Interior Models of Uranus and Neptune
journal, December 2010
- Helled, Ravit; Anderson, John D.; Podolak, Morris
- The Astrophysical Journal, Vol. 726, Issue 1
Chemical processes in the deep interior of Uranus
journal, February 2011
- Chau, Ricky; Hamel, Sebastien; Nellis, William J.
- Nature Communications, Vol. 2, Issue 1
The Interior Structure, Composition, and Evolution of Giant Planets
journal, December 2009
- Fortney, Jonathan J.; Nettelmann, Nadine
- Space Science Reviews, Vol. 152, Issue 1-4
New indication for a dichotomy in the interior structure of Uranus and Neptune from the application of modified shape and rotation data
journal, March 2013
- Nettelmann, N.; Helled, R.; Fortney, J. J.
- Planetary and Space Science, Vol. 77
Superionic and Metallic States of Water and Ammonia at Giant Planet Conditions
journal, January 1999
- Cavazzoni, C.
- Science, Vol. 283, Issue 5398
The Exoplanet Orbit Database
journal, April 2011
- Wright, J. T.; Fakhouri, O.; Marcy, G. W.
- Publications of the Astronomical Society of the Pacific, Vol. 123, Issue 902
VALIDATION OF KEPLER 'S MULTIPLE PLANET CANDIDATES. III. LIGHT CURVE ANALYSIS AND ANNOUNCEMENT OF HUNDREDS OF NEW MULTI-PLANET SYSTEMS
journal, March 2014
- Rowe, Jason F.; Bryson, Stephen T.; Marcy, Geoffrey W.
- The Astrophysical Journal, Vol. 784, Issue 1
The PLATO 2.0 mission
journal, September 2014
- Rauer, H.; Catala, C.; Aerts, C.
- Experimental Astronomy, Vol. 38, Issue 1-2
Water vapour absorption in the clear atmosphere of a Neptune-sized exoplanet
journal, September 2014
- Fraine, Jonathan; Deming, Drake; Benneke, Bjorn
- Nature, Vol. 513, Issue 7519
Magnetic moment and plasma environment of HD 209458b as determined from Ly observations
journal, November 2014
- Kislyakova, K. G.; Holmstrom, M.; Lammer, H.
- Science, Vol. 346, Issue 6212
Diffusion and electrical conductivity in water at ultrahigh pressures
journal, November 2010
- French, Martin; Mattsson, Thomas R.; Redmer, Ronald
- Physical Review B, Vol. 82, Issue 17
The phase diagram of water and the magnetic fields of Uranus and Neptune
journal, January 2011
- Redmer, Ronald; Mattsson, Thomas R.; Nettelmann, Nadine
- Icarus, Vol. 211, Issue 1
Superionic to Superionic Phase Change in Water: Consequences for the Interiors of Uranus and Neptune
journal, April 2013
- Wilson, Hugh F.; Wong, Michael L.; Militzer, Burkhard
- Physical Review Letters, Vol. 110, Issue 15
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
Ab initio simulations of hot dense methane during shock experiments
journal, December 2012
- Sherman, Benjamin L.; Wilson, Hugh F.; Weeraratne, Dayanthie
- Physical Review B, Vol. 86, Issue 22
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 electrical conductivity of “synthetic Uranus,” a mixture of water, ammonia, and isopropanol, at shock pressure up to 200 GPa (2 Mbar)
journal, December 1997
- Nellis, W. J.; Holmes, N. C.; Mitchell, A. C.
- The Journal of Chemical Physics, Vol. 107, Issue 21
Viscosity and stress autocorrelation function in supercooled water: a molecular dynamics study
journal, August 2002
- Guo, Guang-Jun; Zhang, Yi-Gang; Refson, Keith
- Molecular Physics, Vol. 100, Issue 16
A unified formulation of the constant temperature molecular dynamics methods
journal, July 1984
- Nosé, Shuichi
- The Journal of Chemical Physics, Vol. 81, Issue 1
Ab initiomolecular dynamics for liquid metals
journal, January 1993
- Kresse, G.; Hafner, J.
- Physical Review B, Vol. 47, Issue 1, p. 558-561
Ab initio molecular dynamics for open-shell transition metals
journal, November 1993
- Kresse, G.; Hafner, J.
- Physical Review B, Vol. 48, Issue 17
Efficient iterative schemes for ab initio total-energy calculations using a plane-wave basis set
journal, October 1996
- Kresse, G.; Furthmüller, J.
- Physical Review B, Vol. 54, Issue 16, p. 11169-11186
Ab-initio simulations of materials using VASP: Density-functional theory and beyond
journal, October 2008
- Hafner, Jürgen
- Journal of Computational Chemistry, Vol. 29, Issue 13
Inhomogeneous Electron Gas
journal, November 1964
- Hohenberg, P.; Kohn, W.
- Physical Review, Vol. 136, Issue 3B, p. B864-B871
Self-Consistent Equations Including Exchange and Correlation Effects
journal, November 1965
- Kohn, W.; Sham, L. J.
- Physical Review, Vol. 140, Issue 4A, p. A1133-A1138
Fractional occupations and density-functional energies and forces
journal, June 1992
- Weinert, M.; Davenport, J. W.
- Physical Review B, Vol. 45, Issue 23
Energy versus free-energy conservation in first-principles molecular dynamics
journal, May 1992
- Wentzcovitch, Renata M.; Martins, José Luís; Allen, Philip B.
- Physical Review B, Vol. 45, Issue 19
Efficiency of ab-initio total energy calculations for metals and semiconductors using a plane-wave basis set
journal, July 1996
- Kresse, G.; Furthmüller, J.
- Computational Materials Science, Vol. 6, Issue 1, p. 15-50
Projector augmented-wave method
journal, December 1994
- Blöchl, P. E.
- Physical Review B, Vol. 50, Issue 24, p. 17953-17979
From ultrasoft pseudopotentials to the projector augmented-wave method
journal, January 1999
- Kresse, G.; Joubert, D.
- Physical Review B, Vol. 59, Issue 3, p. 1758-1775
Generalized Gradient Approximation Made Simple
journal, October 1996
- Perdew, John P.; Burke, Kieron; Ernzerhof, Matthias
- Physical Review Letters, Vol. 77, Issue 18, p. 3865-3868
Mean-Value Point in the Brillouin Zone
journal, June 1973
- Baldereschi, A.
- Physical Review B, Vol. 7, Issue 12
Thermodynamics and quantum corrections from molecular dynamics for liquid water
journal, September 1983
- Berens, Peter H.; Mackay, Donald H. J.; White, Gary M.
- The Journal of Chemical Physics, Vol. 79, Issue 5
Dissociation of methane under high pressure
journal, October 2010
- Gao, Guoying; Oganov, Artem R.; Ma, Yanming
- The Journal of Chemical Physics, Vol. 133, Issue 14
Probing the Interiors of the Ice Giants: Shock Compression of Water to 700 GPa and
journal, February 2012
- Knudson, M. D.; Desjarlais, M. P.; Lemke, R. W.
- Physical Review Letters, Vol. 108, Issue 9
Inhomogeneous Electron Gas
journal, March 1973
- Rajagopal, A. K.; Callaway, J.
- Physical Review B, Vol. 7, Issue 5
Amorphization-induced surface electronic states modulation of cobaltous oxide nanosheets for lithium-sulfur batteries
journal, May 2021
- Li, Ruilong; Rao, Dewei; Zhou, Jianbin
- Nature Communications, Vol. 12, Issue 1
Reducing Dzyaloshinskii-Moriya interaction and field-free spin-orbit torque switching in synthetic antiferromagnets
journal, May 2021
- Chen, Ruyi; Cui, Qirui; Liao, Liyang
- Nature Communications, Vol. 12, Issue 1
High-resolution X-ray luminescence extension imaging
journal, February 2021
- Ou, Xiangyu; Qin, Xian; Huang, Bolong
- Nature, Vol. 590, Issue 7846
Electronic structure of AlFeN films exhibiting crystallographic orientation change from c- to a-axis with Fe concentrations and annealing effect
journal, February 2020
- Tatemizo, Nobuyuki; Imada, Saki; Okahara, Kizuna
- Scientific Reports, Vol. 10, Issue 1
Molecular Spectra and Molecular Structure
journal, November 1929
- Garner, W. E.; Lennard-Jones, J. E.
- Nature, Vol. 124, Issue 3133
Molecular Spectra and Molecular Structure
journal, October 1929
- Garner, W. E.; Lennard-Jones, J. E.
- Nature, Vol. 124, Issue 3128
The Exoplanet Orbit Database
text, January 2010
- Wright, Jason T.; Fakhouri, Onsi; Marcy, Geoffrey W.
- arXiv
Superionic to superionic phase change in water: consequences for the interiors of Uranus and Neptune
text, January 2012
- Wilson, Hugh F.; Wong, Michael L.; Militzer, Burkhard
- arXiv
Magnetic moment and plasma environment of HD 209458b as determined from Ly$α$ observations
text, January 2014
- Kislyakova, K. G.; Holmström, M.; Lammer, H.
- arXiv
Works referencing / citing this record:
Laser-driven shock compression of “synthetic planetary mixtures” of water, ethanol, and ammonia
journal, July 2019
- Guarguaglini, M.; Hernandez, J. -A.; Okuchi, T.
- Scientific Reports, Vol. 9, Issue 1
Stabilization of ammonia-rich hydrate inside icy planets
journal, August 2017
- Naden Robinson, Victor; Wang, Yanchao; Ma, Yanming
- Proceedings of the National Academy of Sciences, Vol. 114, Issue 34
Structural determination of neutral Co n clusters ( n = 4–10,13) through IR–UV two-color vibrational spectroscopy and DFT calculations
journal, November 2018
- Bakker, J. M.; Jalink, J.; Dieleman, D.
- Journal of Physics: Condensed Matter, Vol. 30, Issue 49
Multicomponent mutual diffusion in the warm, dense matter regime
journal, September 2019
- White, A. J.; Ticknor, C.; Meyer, E. R.
- Physical Review E, Vol. 100, Issue 3
Benchmarking the effective one-component plasma model for warm dense neon and krypton within quantum molecular dynamics simulation
journal, February 2020
- Wang, Zhao-Qi; Tang, Jun; Hou, Yong
- Physical Review E, Vol. 101, Issue 2
Ab initio calculation of thermodynamic potentials and entropies for superionic water
journal, February 2016
- French, Martin; Desjarlais, Michael P.; Redmer, Ronald
- Physical Review E, Vol. 93, Issue 2
Quantum molecular dynamics study on the proton exchange, ionic structures, and transport properties of warm dense hydrogen-deuterium mixtures
journal, June 2018
- Liu, Lei; Li, Zhi-Guo; Dai, Jia-Yu
- Physical Review E, Vol. 97, Issue 6
Planetary Ices and the Linear Mixing Approximation
journal, October 2017
- Bethkenhagen, M.; Meyer, E. R.; Hamel, S.
- The Astrophysical Journal, Vol. 848, Issue 1
Laser-driven shock compression of “synthetic planetary mixtures” of water, ethanol, and ammonia
journal, July 2019
- Guarguaglini, M.; Hernandez, J. -A.; Okuchi, T.
- Scientific Reports, Vol. 9, Issue 1