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Title: Nonempirical Semilocal Free-Energy Density Functional for Matter under Extreme Conditions

Abstract

The potential for density functional calculations to predict the properties of matter under extreme conditions depends crucially upon having a non-empirical approximate free energy functional valid over a wide range of state conditions. Unlike the ground-state case, no such free-energy exchange- correlation (XC) functional exists. We remedy that with systematic construction of a generalized gradient approximation XC free-energy functional based on rigorous constraints, including the free energy gradient expansion. The new functional provides the correct temperature dependence in the slowly varying regime and the correct zero-T, high-T, and homogeneous electron gas limits. Application in Kohn-Sham calculations for hot electrons in a static fcc Aluminum lattice demon- strates the combined magnitude of thermal and gradient effects handled by this functional. Its accuracy in the increasingly important warm dense matter regime is attested by excellent agreement of the calculated deuterium equation of state with reference path integral Monte Carlo results at intermediate and elevated temperatures and by low density Al calculations over a wide T range.

Authors:
 [1];  [2];  [3]
  1. Univ. of Florida, Gainesville, FL (United States). Quantum Theory Project, Dept. of Physics and Dept. of Chemistry; Univ. of Rochester, NY (United States). Lab. for Laser Energetics
  2. Univ. of Florida, Gainesville, FL (United States). Dept. of Physics
  3. Univ. of Florida, Gainesville, FL (United States). Quantum Theory Project, Dept. of Physics and Dept. of Chemistry
Publication Date:
Research Org.:
Univ. of Rochester, NY (United States). Lab. for Laser Energetics
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22); USDOE National Nuclear Security Administration (NNSA)
OSTI Identifier:
1423132
Alternate Identifier(s):
OSTI ID: 1420580; OSTI ID: 1423312
Report Number(s):
2017-224-1373
Journal ID: ISSN 0031-9007; PRLTAO; 2017-224, 2330, 1373; TRN: US1801715
Grant/Contract Number:  
NA0001944; SC0002139
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Physical Review Letters
Additional Journal Information:
Journal Volume: 120; Journal Issue: 7; Journal ID: ISSN 0031-9007
Publisher:
American Physical Society (APS)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSICS

Citation Formats

Karasiev, Valentin V., Dufty, James W., and Trickey, S. B.. Nonempirical Semilocal Free-Energy Density Functional for Matter under Extreme Conditions. United States: N. p., 2018. Web. doi:10.1103/PhysRevLett.120.076401.
Karasiev, Valentin V., Dufty, James W., & Trickey, S. B.. Nonempirical Semilocal Free-Energy Density Functional for Matter under Extreme Conditions. United States. doi:10.1103/PhysRevLett.120.076401.
Karasiev, Valentin V., Dufty, James W., and Trickey, S. B.. Wed . "Nonempirical Semilocal Free-Energy Density Functional for Matter under Extreme Conditions". United States. doi:10.1103/PhysRevLett.120.076401. https://www.osti.gov/servlets/purl/1423132.
@article{osti_1423132,
title = {Nonempirical Semilocal Free-Energy Density Functional for Matter under Extreme Conditions},
author = {Karasiev, Valentin V. and Dufty, James W. and Trickey, S. B.},
abstractNote = {The potential for density functional calculations to predict the properties of matter under extreme conditions depends crucially upon having a non-empirical approximate free energy functional valid over a wide range of state conditions. Unlike the ground-state case, no such free-energy exchange- correlation (XC) functional exists. We remedy that with systematic construction of a generalized gradient approximation XC free-energy functional based on rigorous constraints, including the free energy gradient expansion. The new functional provides the correct temperature dependence in the slowly varying regime and the correct zero-T, high-T, and homogeneous electron gas limits. Application in Kohn-Sham calculations for hot electrons in a static fcc Aluminum lattice demon- strates the combined magnitude of thermal and gradient effects handled by this functional. Its accuracy in the increasingly important warm dense matter regime is attested by excellent agreement of the calculated deuterium equation of state with reference path integral Monte Carlo results at intermediate and elevated temperatures and by low density Al calculations over a wide T range.},
doi = {10.1103/PhysRevLett.120.076401},
journal = {Physical Review Letters},
number = 7,
volume = 120,
place = {United States},
year = {Wed Feb 14 00:00:00 EST 2018},
month = {Wed Feb 14 00:00:00 EST 2018}
}

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