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

Journal Article · · Physical Review Letters
 [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
+ Show Author Affiliations

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.

Research Organization:
Univ. of Rochester, NY (United States). Lab. for Laser Energetics
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES); USDOE National Nuclear Security Administration (NNSA)
Grant/Contract Number:
NA0001944; SC0002139
OSTI ID:
1423312
Alternate ID(s):
OSTI ID: 1420580; OSTI ID: 1423132
Report Number(s):
2017-224-1373; PRLTAO; 2017-224, 2330, 1373; TRN: US1801727
Journal Information:
Physical Review Letters, Vol. 120, Issue 7; ISSN 0031-9007
Publisher:
American Physical Society (APS)Copyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 60 works
Citation information provided by
Web of Science

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A New Model to Predict Optimum Conditions for Growth of 2D Materials on a Substrate journal July 2019

Figures / Tables (7)

FIG. 1(p. 5)figure FIG. 1
FIG. 2(p. 8)figure FIG. 2
FIG. 3(p. 9)figure FIG. 3
FIG. 4(p. 9)figure FIG. 4
TABLE S1(p. 18)table TABLE S1
TABLE S2(p. 21)table TABLE S2
FIG. S1(p. 22)figure FIG. S1

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