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Title: Wannier–Koopmans method calculations for transition metal oxide band gaps

Abstract

The widely used density functional theory (DFT) has a major drawback of underestimating the band gaps of materials. Wannier–Koopmans method (WKM) was recently developed for band gap calculations with accuracy on a par with more complicated methods. WKM has been tested for main group covalent semiconductors, alkali halides, 2D materials, and organic crystals. Here we apply the WKM to another interesting type of material system: the transition metal (TM) oxides. TM oxides can be classified as either with d0 or d10 closed shell occupancy or partially occupied open shell configuration, and the latter is known to be strongly correlated Mott insulators. We found that, while WKM provides adequate band gaps for the d0 and d10 TM oxides, it fails to provide correct band gaps for the group with partially occupied d states. This issue is also found in other mean-field approaches like the GW calculations. We believe that the problem comes from a strong interaction between the occupied and unoccupied d-state Wannier functions in a partially occupied d-state system. We also found that, for pseudopotential calculations including deep core levels, it is necessary to remove the electron densities of these deep core levels in the Hartree and exchange–correlation energy functionalmore » when calculating the WKM correction parameters for the d-state Wannier functions.« less

Authors:
 [1];  [1]; ORCiD logo [2]
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  1. Peking Univ., Shenzhen (China)
  2. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Publication Date:
Research Org.:
Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC)
OSTI Identifier:
1630624
Grant/Contract Number:  
AC02-05CH11231; JCYJ20160226105838578; JCYJ20151015162256516
Resource Type:
Accepted Manuscript
Journal Name:
npj Computational Materials
Additional Journal Information:
Journal Volume: 6; Journal Issue: 1; Journal ID: ISSN 2057-3960
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; computational methods; electronic structure

Citation Formats

Weng, Mouyi, Pan, Feng, and Wang, Lin-Wang. Wannier–Koopmans method calculations for transition metal oxide band gaps. United States: N. p., 2020. Web. doi:10.1038/s41524-020-0302-0.
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Weng, Mouyi, Pan, Feng, & Wang, Lin-Wang. Wannier–Koopmans method calculations for transition metal oxide band gaps. United States. https://doi.org/10.1038/s41524-020-0302-0
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Weng, Mouyi, Pan, Feng, and Wang, Lin-Wang. Fri . "Wannier–Koopmans method calculations for transition metal oxide band gaps". United States. https://doi.org/10.1038/s41524-020-0302-0. https://www.osti.gov/servlets/purl/1630624.
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@article{osti_1630624,
title = {Wannier–Koopmans method calculations for transition metal oxide band gaps},
author = {Weng, Mouyi and Pan, Feng and Wang, Lin-Wang},
abstractNote = {The widely used density functional theory (DFT) has a major drawback of underestimating the band gaps of materials. Wannier–Koopmans method (WKM) was recently developed for band gap calculations with accuracy on a par with more complicated methods. WKM has been tested for main group covalent semiconductors, alkali halides, 2D materials, and organic crystals. Here we apply the WKM to another interesting type of material system: the transition metal (TM) oxides. TM oxides can be classified as either with d0 or d10 closed shell occupancy or partially occupied open shell configuration, and the latter is known to be strongly correlated Mott insulators. We found that, while WKM provides adequate band gaps for the d0 and d10 TM oxides, it fails to provide correct band gaps for the group with partially occupied d states. This issue is also found in other mean-field approaches like the GW calculations. We believe that the problem comes from a strong interaction between the occupied and unoccupied d-state Wannier functions in a partially occupied d-state system. We also found that, for pseudopotential calculations including deep core levels, it is necessary to remove the electron densities of these deep core levels in the Hartree and exchange–correlation energy functional when calculating the WKM correction parameters for the d-state Wannier functions.},
doi = {10.1038/s41524-020-0302-0},
journal = {npj Computational Materials},
number = 1,
volume = 6,
place = {United States},
year = {Fri Apr 03 00:00:00 EDT 2020},
month = {Fri Apr 03 00:00:00 EDT 2020}
}
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Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record
https://doi.org/10.1038/s41524-020-0302-0
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Cited by: 7 works
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Figures / Tables:

Fig. 1 Fig. 1: Band Gap comparison between WKM/LDA calculations and experimental results. Comparing the experimental band gaps against band gap calculated by WKM in SG15 pseudopotential (labeled as SG15-WKM), SG15 pseudopotential with core-level fixation (labeled as SG15-WKM-fix1), FHI pseudopotential (labeled as FHI–WKM) and LDA with SG15 (labeled as SG15-LDA) and FHImore » (labeled as FHI–LDA) pseudopotential.« less
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Works referenced in this record:

Using Wannier functions to improve solid band gap predictions in density functional theory
journal, April 2016

Insights and challenges of applying the GW method to transition metal oxides
journal, October 2014

Density-functional calculation of effective Coulomb interactions in metals
journal, April 1991

Hybrid functionals based on a screened Coulomb potential
journal, May 2003

  • Heyd, Jochen; Scuseria, Gustavo E.; Ernzerhof, Matthias
  • The Journal of Chemical Physics, Vol. 118, Issue 18
  • DOI: 10.1063/1.1564060

Efficiency of ab-initio total energy calculations for metals and semiconductors using a plane-wave basis set
journal, July 1996

Electronic structure of MnO
journal, July 1991

Ab initio pseudopotentials for electronic structure calculations of poly-atomic systems using density-functional theory
journal, June 1999

TiO 2 Anatase with a Bandgap in the Visible Region
journal, October 2014

  • Dette, Christian; Pérez-Osorio, Miguel A.; Kley, Christopher S.
  • Nano Letters, Vol. 14, Issue 11
  • DOI: 10.1021/nl503131s

The analysis of a plane wave pseudopotential density functional theory code on a GPU machine
journal, January 2013

Wannier Koopmans Method Calculations of 2D Material Band Gaps
journal, January 2018

A new local density functional for main-group thermochemistry, transition metal bonding, thermochemical kinetics, and noncovalent interactions
journal, November 2006

  • Zhao, Yan; Truhlar, Donald G.
  • The Journal of Chemical Physics, Vol. 125, Issue 19, Article No. 194101
  • DOI: 10.1063/1.2370993

Fast plane wave density functional theory molecular dynamics calculations on multi-GPU machines
journal, October 2013

Testing variations of the GW approximation on strongly correlated transition metal oxides: hematite (α-Fe2O3) as a benchmark
journal, January 2011

  • Liao, Peilin; Carter, Emily A.
  • Physical Chemistry Chemical Physics, Vol. 13, Issue 33
  • DOI: 10.1039/c1cp20829b

Commentary: The Materials Project: A materials genome approach to accelerating materials innovation
journal, July 2013

  • Jain, Anubhav; Ong, Shyue Ping; Hautier, Geoffroy
  • APL Materials, Vol. 1, Issue 1
  • DOI: 10.1063/1.4812323

Band-structure calculations for the 3 d transition metal oxides in G W
journal, February 2013

Proof that ∂ E ∂ n i = ε in density-functional theory
journal, December 1978

"Special points for Brillouin-zone integrations"—a reply
journal, August 1977

Optimized norm-conserving Vanderbilt pseudopotentials
journal, August 2013

Wannier Koopman method calculations of the band gaps of alkali halides
journal, July 2017

  • Weng, Mouyi; Li, Sibai; Ma, Jie
  • Applied Physics Letters, Vol. 111, Issue 5
  • DOI: 10.1063/1.4996743

The fundamental absorption edge of AlAs and AlP
journal, May 1970

Comparison of Density Functional and MP2 Calculations on the Water Monomer and Dimer
journal, October 1994

  • Kim, K.; Jordan, K. D.
  • The Journal of Physical Chemistry, Vol. 98, Issue 40
  • DOI: 10.1021/j100091a024

Ionization Potential, Electron Affinity, Electronegativity, Hardness, and Electron Excitation Energy:  Molecular Properties from Density Functional Theory Orbital Energies
journal, May 2003

  • Zhan, Chang-Guo; Nichols, Jeffrey A.; Dixon, David A.
  • The Journal of Physical Chemistry A, Vol. 107, Issue 20
  • DOI: 10.1021/jp0225774

All-Electron Self-Consistent G W Approximation: Application to Si, MnO, and NiO
journal, September 2004

Optimization algorithm for the generation of ONCV pseudopotentials
journal, November 2015

Localized orbital scaling correction for systematic elimination of delocalization error in density functional approximations
journal, September 2017

  • Li, Chen; Zheng, Xiao; Su, Neil Qiang
  • National Science Review, Vol. 5, Issue 2
  • DOI: 10.1093/nsr/nwx111

Dynamical and anharmonic effects on the electron-phonon coupling and the zero-point renormalization of the electronic structure
journal, August 2015

Ab Initio Calculation of Vibrational Absorption and Circular Dichroism Spectra Using Density Functional Force Fields
journal, November 1994

  • Stephens, P. J.; Devlin, F. J.; Chabalowski, C. F.
  • The Journal of Physical Chemistry, Vol. 98, Issue 45, p. 11623-11627
  • DOI: 10.1021/j100096a001

Piecewise Linearity of Approximate Density Functionals Revisited: Implications for Frontier Orbital Energies
journal, March 2013

Compilation of Energy Band Gaps in Elemental and Binary Compound Semiconductors and Insulators
journal, January 1973

  • Strehlow, W. H.; Cook, E. L.
  • Journal of Physical and Chemical Reference Data, Vol. 2, Issue 1
  • DOI: 10.1063/1.3253115

Thin‐film modeling for mechanical measurements: Should membranes be used or plates?
journal, May 1992

  • Fartash, A.; Schuller, Ivan K.; Grimsditch, M.
  • Journal of Applied Physics, Vol. 71, Issue 9
  • DOI: 10.1063/1.350804

Convergence of quasiparticle self-consistent G W calculations of transition-metal monoxides
journal, March 2015

Self-Consistent Equations Including Exchange and Correlation Effects
journal, November 1965

Linear response approach to the calculation of the effective interaction parameters in the LDA + U method
journal, January 2005

Density-functional theory calculations for poly-atomic systems: electronic structure, static and elastic properties and ab initio molecular dynamics
journal, December 1997

TiO 2 Anatase with a Bandgap in the Visible Region
journal, October 2014

  • Dette, Christian; Pérez-Osorio, Miguel A.; Kley, Christopher S.
  • Nano Letters, Vol. 14, Issue 11
  • DOI: 10.1021/nl503131s

Thin‐film modeling for mechanical measurements: Should membranes be used or plates?
journal, May 1992

  • Fartash, A.; Schuller, Ivan K.; Grimsditch, M.
  • Journal of Applied Physics, Vol. 71, Issue 9
  • DOI: 10.1063/1.350804

Maximally localized Wannier functions for entangled energy bands
journal, December 2001

Optimization Algorithm for the Generation of ONCV Pseudopotentials
text, January 2015

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