Thermodynamic properties of ε-Fe with thermal electronic excitation effects on vibrational spectra
Abstract
The thermodynamic properties of hexagonal-close-packed iron (ε–Fe) are essential for investigating the internal structure and dynamic properties of planetary cores. Despite their importance to planetary sciences, experimental investigations of ε–Fe at relevant conditions are still challenging. Therefore, ab initio calculations are crucial to elucidating the thermodynamic properties of this system. Here, we use a free energy calculation scheme based on the phonon gas model compatible with temperature-dependent phonon frequencies. We investigate the effects of electronic thermal excitations, which introduces a temperature dependence on phonon frequencies, and the implication for the thermodynamic properties of ε–Fe at extreme pressure (P) and temperature (T) conditions. We disregard phonon-phonon interactions, i.e., anharmonicity and their effect on phonon frequencies. Nevertheless, the current scheme is also applicable to T -dependent anharmonic frequencies. We conclude that the impact of thermal electronic excitations on vibrational properties is not significant up to ~4000 K at 200 GPa but should not be ignored at higher temperatures or pressures. However, the static free energy Fst must always include the effect of thermal excitation fully in a continuum of T. Furthermore, our results for isentropic equations of state show good agreement with data from recent ramp compression experiments up to 1400 GPamore »
- Authors:
-
[1]
- Columbia Univ., New York, NY (United States); Columbia Univ., Palisades, NY (United States)
- Columbia Univ., New York, NY (United States)
- Publication Date:
- Research Org.:
- Columbia Univ., New York, NY (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC); National Science Foundation (NSF)
- OSTI Identifier:
- 1853389
- Grant/Contract Number:
- SC0019759; EAR-1918126; ACI-1548562; ACI-1134872
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Physical Review. B
- Additional Journal Information:
- Journal Volume: 103; Journal Issue: 14; Journal ID: ISSN 2469-9950
- Publisher:
- American Physical Society (APS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY; Materials Science; Physics; Phonons; Pressure effects; Thermodynamics of computation; Metals; Density functional theory; First-principles calculations
Citation Formats
Zhuang, Jingyi, Wang, Hongjin, Zhang, Qi, and Wentzcovitch, Renata M. Thermodynamic properties of ε-Fe with thermal electronic excitation effects on vibrational spectra. United States: N. p., 2021.
Web. doi:10.1103/physrevb.103.144102.
Zhuang, Jingyi, Wang, Hongjin, Zhang, Qi, & Wentzcovitch, Renata M. Thermodynamic properties of ε-Fe with thermal electronic excitation effects on vibrational spectra. United States. https://doi.org/10.1103/physrevb.103.144102
Zhuang, Jingyi, Wang, Hongjin, Zhang, Qi, and Wentzcovitch, Renata M. Mon .
"Thermodynamic properties of ε-Fe with thermal electronic excitation effects on vibrational spectra". United States. https://doi.org/10.1103/physrevb.103.144102. https://www.osti.gov/servlets/purl/1853389.
@article{osti_1853389,
title = {Thermodynamic properties of ε-Fe with thermal electronic excitation effects on vibrational spectra},
author = {Zhuang, Jingyi and Wang, Hongjin and Zhang, Qi and Wentzcovitch, Renata M.},
abstractNote = {The thermodynamic properties of hexagonal-close-packed iron (ε–Fe) are essential for investigating the internal structure and dynamic properties of planetary cores. Despite their importance to planetary sciences, experimental investigations of ε–Fe at relevant conditions are still challenging. Therefore, ab initio calculations are crucial to elucidating the thermodynamic properties of this system. Here, we use a free energy calculation scheme based on the phonon gas model compatible with temperature-dependent phonon frequencies. We investigate the effects of electronic thermal excitations, which introduces a temperature dependence on phonon frequencies, and the implication for the thermodynamic properties of ε–Fe at extreme pressure (P) and temperature (T) conditions. We disregard phonon-phonon interactions, i.e., anharmonicity and their effect on phonon frequencies. Nevertheless, the current scheme is also applicable to T -dependent anharmonic frequencies. We conclude that the impact of thermal electronic excitations on vibrational properties is not significant up to ~4000 K at 200 GPa but should not be ignored at higher temperatures or pressures. However, the static free energy Fst must always include the effect of thermal excitation fully in a continuum of T. Furthermore, our results for isentropic equations of state show good agreement with data from recent ramp compression experiments up to 1400 GPa conducted at the National Ignition Facility.},
doi = {10.1103/physrevb.103.144102},
journal = {Physical Review. B},
number = 14,
volume = 103,
place = {United States},
year = {Mon Apr 12 00:00:00 EDT 2021},
month = {Mon Apr 12 00:00:00 EDT 2021}
}
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