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Assessing the source of error in the Thomas–Fermi–von Weizsäcker density functional

Journal Article · · Journal of Chemical Physics
DOI:https://doi.org/10.1063/5.0146167· OSTI ID:1988164
 [1];  [2];  [3];  [2];  [4]
  1. George Mason University, Fairfax, VA (United States); Georgia Institute of Technology
  2. Georgia Institute of Technology, Atlanta, GA (United States)
  3. Lawrence Livermore National Laboratory (LLNL), Livermore, CA (United States)
  4. George Mason University, Fairfax, VA (United States)
+ Show Author Affiliations
We investigate the source of error in the Thomas–Fermi–von Weizsäcker (TFW) density functional relative to Kohn–Sham density functional theory (DFT). In particular, through numerical studies on a range of materials, for a variety of crystal structures subject to strain and atomic displacements, we find that while the ground state electron density in TFW orbital-free DFT is close to the Kohn–Sham density, the corresponding energy deviates significantly from the Kohn–Sham value. Here, we show that these differences are a consequence of the poor representation of the linear response within the TFW approximation for the electronic kinetic energy, confirming conjectures in the literature. In so doing, we find that the energy computed from a non-self-consistent Kohn–Sham calculation using the TFW electronic ground state density is in very good agreement with that obtained from the fully self-consistent Kohn–Sham solution.
Research Organization:
Georgia Institute of Technology, Atlanta, GA (United States); Lawrence Livermore National Laboratory (LLNL), Livermore, CA (United States)
Sponsoring Organization:
USDOE National Nuclear Security Administration (NNSA); USDOE Office of Science (SC); USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division (CSGB)
Grant/Contract Number:
AC52-07NA27344; SC0019410
OSTI ID:
1988164
Alternate ID(s):
OSTI ID: 2204474
Report Number(s):
LLNL--JRNL-856375
Journal Information:
Journal of Chemical Physics, Journal Name: Journal of Chemical Physics Journal Issue: 21 Vol. 158; ISSN 0021-9606
Publisher:
American Institute of Physics (AIP)Copyright Statement
Country of Publication:
United States
Language:
English

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Related Subjects

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
Bosons
Crystal structure
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Local density approximations
Phonons
Quantum chemistry
Self consistent field methods