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Title: Electronic properties of doped and defective NiO: A quantum Monte Carlo study

Journal Article · · Physical Review Materials
 [1];  [1]; ORCiD logo [2]; ORCiD logo [2]; ORCiD logo [3]; ORCiD logo [2];  [1];  [4]
  1. Argonne National Lab. (ANL), Argonne, IL (United States)
  2. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Science (CNMS)
  3. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Materials Science & Technology Division
  4. Argonne National Lab. (ANL), Argonne, IL (United States). Materials Science Division; Northwestern Univ., Evanston, IL (United States). Inst. for Science and Engineering
+ Show Author Affiliations

NiO is a canonical Mott (or charge-transfer) insulator and, as such, is notoriously difficult to describe using density functional theory (DFT)–based electronic structure methods. Doped Mott insulators such as NiO are of interest for various applications but rigorous theoretical descriptions are lacking. Here, we use quantum Monte Carlo methods, which very accurately include electron-electron interactions, to examine energetics, charge structures, and spin structures of NiO with various point defects, such as vacancies and substitutional doping with potassium. The formation energy of a potassium dopant is significantly lower than that of a Ni vacancy, making potassium an attractive monovalent dopant for NiO. We compare our results with DFT results that include an on-site Hubbard U (DFT+U) to account for correlations and find relatively large discrepancies for defect formation energies as well as for charge and spin redistributions in the presence of point defects. Beyond fitting to a single property, it is unlikely that single-parameter tuning of the DFT+U will be able to obtain accurate accounts of complex properties in these materials. Responses that depend in subtle and complex ways on ground-state properties, such as charge and spin densities, are likely to contain quantitative and qualitative errors.

Research Organization:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Oak Ridge Leadership Computing Facility (OLCF); Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Materials Sciences & Engineering Division; USDOE Office of Science (SC), Basic Energy Sciences (BES)
Grant/Contract Number:
AC02-06CH11357; AC05-00OR22725; AC02-05CH11231
OSTI ID:
1416980
Alternate ID(s):
OSTI ID: 1416430; OSTI ID: 1422575
Journal Information:
Physical Review Materials, Vol. 1, Issue 7; ISSN 2475-9953
Publisher:
American Physical Society (APS)Copyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 31 works
Citation information provided by
Web of Science

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  • Osorio-Guillén, Jorge; Lany, Stephan; Zunger, Alex
  • PHYSICS OF SEMICONDUCTORS: 29th International Conference on the Physics of Semiconductors, AIP Conference Proceedings https://doi.org/10.1063/1.3295330
conference January 2010
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Cited By (10)

Identification and modulation of electronic band structures of single-phase β-(Al x Ga 1−x ) 2 O 3 alloys grown by laser molecular beam epitaxy journal July 2018
An efficient hybrid orbital representation for quantum Monte Carlo calculations journal August 2018
Auxiliary-field quantum Monte Carlo calculations of the structural properties of nickel oxide journal October 2018
A new scheme for fixed node diffusion quantum Monte Carlo with pseudopotentials: Improving reproducibility and reducing the trial-wave-function bias journal October 2019
Diffusion Monte Carlo study of O 2 adsorption on single layer graphene journal August 2019
Defect energetics of cubic hafnia from quantum Monte Carlo simulations journal July 2019
Structural, electronic, and magnetic properties of bulk and epitaxial LaCoO 3 through diffusion Monte Carlo journal December 2019
QMCPACK : An open source ab initio Quantum Monte Carlo package for the electronic structure of atoms, molecules, and solids text January 2018
An efficient hybrid orbital representation for quantum Monte Carlo calculations text January 2018
Defect energetics of cubic hafnia from quantum Monte Carlo simulations text January 2019

Figures / Tables (14)

FIG. 2(p. 8)figure FIG. 2
FIG. 3(p. 8)figure FIG. 3
Table I(p. 9)table Table I
FIG. 4(p. 11)figure FIG. 4
FIG. 5(p. 12)figure FIG. 5
Table II(p. 13)table Table II
FIG. 6(p. 14)figure FIG. 6
FIG. 7(p. 16)figure FIG. 7
FIG. 8(p. 16)figure FIG. 8
Table III(p. 17)table Table III
Table IV(p. 20)table Table IV
FIG. 9(p. 21)figure FIG. 9
FIG. 10(p. 22)figure FIG. 10
FIG. 11(p. 22)figure FIG. 11

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36 MATERIALS SCIENCE
Quantum Monte Carlo
Density Functional Theory
DFT
Point Defects