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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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