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Title: Many-body ab initio diffusion quantum Monte Carlo applied to the strongly correlated oxide NiO

Abstract

We present a many-body diffusion quantum Monte Carlo (DMC) study of the bulk and defect properties of NiO. We find excellent agreement with experimental values, within 0.3%, 0.6%, and 3.5% for the lattice constant, cohesive energy, and bulk modulus, respectively. The quasiparticle bandgap was also computed, and the DMC result of 4.72 (0.17) eV compares well with the experimental value of 4.3 eV. Furthermore, DMC calculations of excited states at the L, Z, and the gamma point of the Brillouin zone reveal a flat upper valence band for NiO, in good agreement with Angle Resolved Photoemission Spectroscopy results. To study defect properties, we evaluated the formation energies of the neutral and charged vacancies of oxygen and nickel in NiO. A formation energy of 7.2 (0.15) eV was found for the oxygen vacancy under oxygen rich conditions. For the Ni vacancy, we obtained a formation energy of 3.2 (0.15) eV under Ni rich conditions. Lastly, these results confirm that NiO occurs as a p-type material with the dominant intrinsic vacancy defect being Ni vacancy.

Authors:
 [1];  [1]; ORCiD logo [1];  [1]
  1. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Materials Science and Technology Division
Publication Date:
Research Org.:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Oak Ridge Leadership Computing Facility (OLCF)
Sponsoring Org.:
DOE Office of Science (SC)
OSTI Identifier:
1329128
Grant/Contract Number:  
AC05-00OR22725
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Chemical Physics
Additional Journal Information:
Journal Volume: 143; Journal Issue: 16; Journal ID: ISSN 0021-9606
Publisher:
American Institute of Physics (AIP)
Country of Publication:
United States
Language:
English
Subject:
71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSICS; 97 MATHEMATICS AND COMPUTING; nickel; vacancies; Laser Doppler velocimetry; band gap; collective excitations

Citation Formats

Mitra, Chandrima, Krogel, Jaron T., Santana, Juan A., and Reboredo, Fernando A. Many-body ab initio diffusion quantum Monte Carlo applied to the strongly correlated oxide NiO. United States: N. p., 2015. Web. doi:10.1063/1.4934262.
Mitra, Chandrima, Krogel, Jaron T., Santana, Juan A., & Reboredo, Fernando A. Many-body ab initio diffusion quantum Monte Carlo applied to the strongly correlated oxide NiO. United States. doi:10.1063/1.4934262.
Mitra, Chandrima, Krogel, Jaron T., Santana, Juan A., and Reboredo, Fernando A. Wed . "Many-body ab initio diffusion quantum Monte Carlo applied to the strongly correlated oxide NiO". United States. doi:10.1063/1.4934262. https://www.osti.gov/servlets/purl/1329128.
@article{osti_1329128,
title = {Many-body ab initio diffusion quantum Monte Carlo applied to the strongly correlated oxide NiO},
author = {Mitra, Chandrima and Krogel, Jaron T. and Santana, Juan A. and Reboredo, Fernando A.},
abstractNote = {We present a many-body diffusion quantum Monte Carlo (DMC) study of the bulk and defect properties of NiO. We find excellent agreement with experimental values, within 0.3%, 0.6%, and 3.5% for the lattice constant, cohesive energy, and bulk modulus, respectively. The quasiparticle bandgap was also computed, and the DMC result of 4.72 (0.17) eV compares well with the experimental value of 4.3 eV. Furthermore, DMC calculations of excited states at the L, Z, and the gamma point of the Brillouin zone reveal a flat upper valence band for NiO, in good agreement with Angle Resolved Photoemission Spectroscopy results. To study defect properties, we evaluated the formation energies of the neutral and charged vacancies of oxygen and nickel in NiO. A formation energy of 7.2 (0.15) eV was found for the oxygen vacancy under oxygen rich conditions. For the Ni vacancy, we obtained a formation energy of 3.2 (0.15) eV under Ni rich conditions. Lastly, these results confirm that NiO occurs as a p-type material with the dominant intrinsic vacancy defect being Ni vacancy.},
doi = {10.1063/1.4934262},
journal = {Journal of Chemical Physics},
number = 16,
volume = 143,
place = {United States},
year = {2015},
month = {10}
}

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Works referenced in this record:

Quasiparticle energy bands of transition-metal oxides within a model GW scheme
journal, May 1997


First-principles modeling of localized d states with the G W @ LDA + U approach
journal, July 2010


First-principles calculation of NiO valence spectra in the impurity-Anderson-model approximation
journal, September 1994

  • Anisimov, Vladimir I.; Kuiper, Pieter; Nordgren, Joseph
  • Physical Review B, Vol. 50, Issue 12
  • DOI: 10.1103/PhysRevB.50.8257

Projector augmented-wave method
journal, December 1994


LDA + DMFT computation of the electronic spectrum of NiO
journal, November 2006


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

Band gaps and electronic structure of transition-metal compounds
journal, July 1985


Quantum Monte Carlo simulations of solids
journal, January 2001


QUANTUM ESPRESSO: a modular and open-source software project for quantum simulations of materials
journal, September 2009

  • Giannozzi, Paolo; Baroni, Stefano; Bonini, Nicola
  • Journal of Physics: Condensed Matter, Vol. 21, Issue 39, Article No. 395502
  • DOI: 10.1088/0953-8984/21/39/395502

Ab initio Quantum Monte Carlo Calculations of Spin Superexchange in Cuprates: The Benchmarking Case of Ca 2 CuO 3
journal, July 2014


Reproducible resistance switching in polycrystalline NiO films
journal, December 2004

  • Seo, S.; Lee, M. J.; Seo, D. H.
  • Applied Physics Letters, Vol. 85, Issue 23
  • DOI: 10.1063/1.1831560

Electron-energy-loss spectra and the structural stability of nickel oxide: An LSDA+U study
journal, January 1998

  • Dudarev, S. L.; Botton, G. A.; Savrasov, S. Y.
  • Physical Review B, Vol. 57, Issue 3, p. 1505-1509
  • DOI: 10.1103/PhysRevB.57.1505

Periodic boundary conditions in ab initio calculations
journal, February 1995


Point defects in sputtered NiO films
journal, February 2009

  • Jang, Wei-Luen; Lu, Yang-Ming; Hwang, Weng-Sing
  • Applied Physics Letters, Vol. 94, Issue 6
  • DOI: 10.1063/1.3081025

Quantum Monte Carlo calculations for ground and excited states
journal, November 2001

  • Needs, R. J.; Kent, P. R. C.; Porter, A. R.
  • International Journal of Quantum Chemistry, Vol. 86, Issue 2
  • DOI: 10.1002/qua.1602

Quantum Monte Carlo applied to solids
journal, December 2013


Structural stability and defect energetics of ZnO from diffusion quantum Monte Carlo
journal, April 2015

  • Santana, Juan A.; Krogel, Jaron T.; Kim, Jeongnim
  • The Journal of Chemical Physics, Vol. 142, Issue 16
  • DOI: 10.1063/1.4919242

Norm-Conserving Pseudopotentials
journal, November 1979


The Compressibility of Media under Extreme Pressures
journal, September 1944

  • Murnaghan, F. D.
  • Proceedings of the National Academy of Sciences, Vol. 30, Issue 9
  • DOI: 10.1073/pnas.30.9.244

NiO: Correlated Band Structure of a Charge-Transfer Insulator
journal, October 2007


Finite-size effects and Coulomb interactions in quantum Monte Carlo calculations for homogeneous systems with periodic boundary conditions
journal, January 1996


Correlation between electrical properties and point defects in NiO thin films
journal, December 2012

  • Kwon, Yong Hun; Chun, Sung Hyun; Han, Jae-Hee
  • Metals and Materials International, Vol. 18, Issue 6
  • DOI: 10.1007/s12540-012-6012-5

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


Interaction and ordering of vacancy defects in NiO
journal, April 2008


Defect energetics in ZnO: A hybrid Hartree-Fock density functional study
journal, June 2008


Multielectron satellites and spin polarization in photoemission from Ni compounds
journal, May 1984


Magnetic ordering and exchange effects in the antiferromagnetic solid solutions Mn x Ni 1 x O
journal, June 1983


Finite-Size Error in Many-Body Simulations with Long-Range Interactions
journal, August 2006


The Basis of the Electron Theory of Metals, with Special Reference to the Transition Metals
journal, July 1949


Nexus: A modular workflow management system for quantum simulation codes
journal, January 2016


Elimination of Coulomb finite-size effects in quantum many-body simulations
journal, February 1997


Linear Response Calculations of Lattice Dynamics in Strongly Correlated Systems
journal, February 2003


Accurate screened exchange band structures for the transition metal monoxides MnO, FeO, CoO and NiO
journal, April 2013


Electronic Structure of NiO in the GW Approximation
journal, April 1995


Finite-size errors in continuum quantum Monte Carlo calculations
journal, September 2008


Quasiparticle energy bands of NiO in the G W approximation
journal, May 2005


The energy and elastic dipole tensor of defects in ionic crystals calculated by the supercell method
journal, February 1985


THE DIFFUSION QUANTUM MONTE CARLO METHOD: DESIGNING TRIAL WAVE FUNCTIONS FOR NiO
journal, November 2003


Use of thermionic emission for studying of point defects in NiO single crystals
journal, June 1984


Cohesive Energy of NiO: A Quantum Monte Carlo Approach
journal, June 1993

  • Tanaka, Shigenori
  • Journal of the Physical Society of Japan, Vol. 62, Issue 6
  • DOI: 10.1143/JPSJ.62.2112

Efficient iterative schemes for ab initio total-energy calculations using a plane-wave basis set
journal, October 1996


Chemical potential dependence of defect formation energies in GaAs: Application to Ga self-diffusion
journal, October 1991


Ab initio molecular-dynamics simulation of the liquid-metal–amorphous-semiconductor transition in germanium
journal, May 1994


First-principles calculations for point defects in solids
journal, March 2014

  • Freysoldt, Christoph; Grabowski, Blazej; Hickel, Tilmann
  • Reviews of Modern Physics, Vol. 86, Issue 1
  • DOI: 10.1103/RevModPhys.86.253

Band theory and Mott insulators: Hubbard U instead of Stoner I
journal, July 1991

  • Anisimov, Vladimir I.; Zaanen, Jan; Andersen, Ole K.
  • Physical Review B, Vol. 44, Issue 3, p. 943-954
  • DOI: 10.1103/PhysRevB.44.943

Covalency Parameters in MnO, α‐MnS, and NiO
journal, February 1968

  • Fender, B. E. F.; Jacobson, A. J.; Wedgwood, F. A.
  • The Journal of Chemical Physics, Vol. 48, Issue 3
  • DOI: 10.1063/1.1668855

Ground State of the Electron Gas by a Stochastic Method
journal, August 1980


Magnitude and Origin of the Band Gap in NiO
journal, December 1984


Twist-averaged boundary conditions in continuum quantum Monte Carlo algorithms
journal, June 2001


Self-interaction correction to density-functional approximations for many-electron systems
journal, May 1981


Transition-metal oxides in the self-interaction–corrected density-functional formalism
journal, August 1990


Diffusion quantum Monte Carlo calculations of the excited states of silicon
journal, May 1998


Quasiparticle band structures of the antiferromagnetic transition-metal oxides MnO, FeO, CoO, and NiO
journal, June 2009


Electronic structure of NiO: Correlation and band effects
journal, August 1991


Continuum variational and diffusion quantum Monte Carlo calculations
journal, December 2009


Optimized pseudopotentials
journal, January 1990

  • Rappe, Andrew M.; Rabe, Karin M.; Kaxiras, Efthimios
  • Physical Review B, Vol. 41, Issue 2
  • DOI: 10.1103/PhysRevB.41.1227

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


Beyond the locality approximation in the standard diffusion Monte Carlo method
journal, October 2006


Band theory of insulating transition-metal monoxides: Band-structure calculations
journal, October 1984


    Works referencing / citing this record:

    Cohesive energy and structural parameters of binary oxides of groups IIA and IIIB from diffusion quantum Monte Carlo
    journal, May 2016

    • Santana, Juan A.; Krogel, Jaron T.; Kent, Paul R. C.
    • The Journal of Chemical Physics, Vol. 144, Issue 17
    • DOI: 10.1063/1.4947569

    Quantitative estimation of localization errors of 3 d transition metal pseudopotentials in diffusion Monte Carlo
    journal, July 2017

    • Dzubak, Allison L.; Krogel, Jaron T.; Reboredo, Fernando A.
    • The Journal of Chemical Physics, Vol. 147, Issue 2
    • DOI: 10.1063/1.4991414

    Auxiliary-field quantum Monte Carlo calculations of the structural properties of nickel oxide
    journal, October 2018

    • Zhang, Shuai; Malone, Fionn D.; Morales, Miguel A.
    • The Journal of Chemical Physics, Vol. 149, Issue 16
    • DOI: 10.1063/1.5040900

    Screened range-separated hybrid by balancing the compact and slowly varying density regimes: Satisfaction of local density linear response
    journal, January 2020

    • Jana, Subrata; Patra, Abhilash; Constantin, Lucian A.
    • The Journal of Chemical Physics, Vol. 152, Issue 4
    • DOI: 10.1063/1.5131530

    Discovering correlated fermions using quantum Monte Carlo
    journal, August 2016


    Phase stability of TiO 2 polymorphs from diffusion Quantum Monte Carlo
    journal, November 2016


    Electronic band gaps from quantum Monte Carlo methods
    journal, February 2020


    Pseudopotentials for quantum Monte Carlo studies of transition metal oxides
    journal, February 2016


    Quantum Monte Carlo calculations of energy gaps from first principles
    journal, August 2018


    Electronic properties of doped and defective NiO: A quantum Monte Carlo study
    journal, December 2017


    Local structure of potassium doped nickel oxide: A combined experimental-theoretical study
    journal, November 2019


    Structural, electronic, and magnetic properties of bulk and epitaxial LaCoO 3 through diffusion Monte Carlo
    journal, December 2019