skip to main content
OSTI.GOV title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: Electron correlation by polarization of interacting densities

Authors:
ORCiD logo [1]
  1. Department of Chemistry, North Carolina State University, Raleigh, North Carolina 27695, USA
Publication Date:
Sponsoring Org.:
USDOE
OSTI Identifier:
1361766
Resource Type:
Journal Article: Publisher's Accepted Manuscript
Journal Name:
Journal of Chemical Physics
Additional Journal Information:
Journal Volume: 146; Journal Issue: 6; Related Information: CHORUS Timestamp: 2018-02-14 19:56:24; Journal ID: ISSN 0021-9606
Publisher:
American Institute of Physics
Country of Publication:
United States
Language:
English

Citation Formats

Whitten, Jerry L. Electron correlation by polarization of interacting densities. United States: N. p., 2017. Web. doi:10.1063/1.4975329.
Whitten, Jerry L. Electron correlation by polarization of interacting densities. United States. doi:10.1063/1.4975329.
Whitten, Jerry L. Tue . "Electron correlation by polarization of interacting densities". United States. doi:10.1063/1.4975329.
@article{osti_1361766,
title = {Electron correlation by polarization of interacting densities},
author = {Whitten, Jerry L.},
abstractNote = {},
doi = {10.1063/1.4975329},
journal = {Journal of Chemical Physics},
number = 6,
volume = 146,
place = {United States},
year = {Tue Feb 14 00:00:00 EST 2017},
month = {Tue Feb 14 00:00:00 EST 2017}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record at 10.1063/1.4975329

Citation Metrics:
Cited by: 1work
Citation information provided by
Web of Science

Save / Share:
  • Here, diffusion quantum Monte Carlo results are used as a reference to analyze properties related to phase stability and magnetism in vanadium dioxide computed with various formulations of density functional theory. We introduce metrics related to energetics, electron densities and spin densities that give us insight on both local and global variations in the antiferromagnetic M1 and R phases. Importantly, these metrics can address contributions arising from the challenging description of the 3d orbital physics in this material. We observe that the best description of energetics between the structural phases does not correspond to the best accuracy in the charge density, which is consistent with observations made recently by Medvedev et~al. in the context of isolated atoms. However, we do find evidence that an accurate spin density connects to correct energetic ordering of different magnetic states in VOmore » $$_2$$, although local, semilocal, and meta-GGA functionals tend to erroneously favor demagnetization of the vanadium sites. The recently developed SCAN functional stands out as remaining nearly balanced in terms of magnetization across the M1-R transition and correctly predicting the ground state crystal structure. In addition to ranking current density functionals, our reference energies and densities serve as important benchmarks for future functional development.« less
  • iffusion quantum Monte Carlo results are used as a reference to analyze properties related to phase stability and magnetism in vanadium dioxide computed with various formulations of density functional theory. We introduce metrics related to energetics, electron densities and spin densities that give us insight on both local and global variations in the antiferromagnetic M1 and R phases. Importantly, these metrics can address contributions arising from the challenging description of the 3d orbital physics in this material. We observe that the best description of energetics between the structural phases does not correspond to the best accuracy in the charge density,more » which is consistent with observations made recently by Medvedev et al. [Science 355, 371 (2017)] in the context of isolated atoms. However, we do find evidence that an accurate spin density connects to correct energetic ordering of different magnetic states in VO2, although local, semilocal, and meta-GGA functionals tend to erroneously favor demagnetization of the vanadium sites. The recently developed SCAN functional stands out as remaining nearly balanced in terms of magnetization across the M1-R transition and correctly predicting the ground state crystal structure. In addition to ranking current density functionals, our reference energies and densities serve as important benchmarks for future functional development. With our reference data, the accuracy of both the energy and the electron density can be monitored simultaneously, which is useful for functional development. So far, this kind of detailed high accuracy reference data for correlated materials has been absent from the literature.« less