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Title: Diffusion Monte Carlo: A pathway towards an accurate theoretical description of manganese oxides

Here, we present diffusion Monte Carlo (DMC) results for equation of state and quasiparticle gaps of manganese binary oxides MnO and MnO 2 and the ternary oxide LaMnO 3. Owing to the limited approximations made and the direct treatment of electronic correlations, our DMC-based study correctly describes structural properties such as the lattice constant, bulk moduli, and cohesive energies. It correctly predicts the ground-state phase of these oxides, which have different valences. Our study demonstrates the capability of DMC methods to predict the structural properties of highly correlated systems, which have been identified as suitable candidates for many applications ranging from catalysis to electronic devices. Our study also serves as a benchmark for both the manganese pseudopotential and other methodological choices to be used in calculations of similar oxides.
Authors:
ORCiD logo [1] ; ORCiD logo [1] ; ORCiD logo [2] ; ORCiD logo [1]
  1. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Materials Science & Technology Division
  2. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Science (CNMS) and Computational Science and Engineering Division
Publication Date:
Grant/Contract Number:
AC05-00OR22725
Type:
Accepted Manuscript
Journal Name:
Physical Review Materials
Additional Journal Information:
Journal Volume: 2; Journal Issue: 8; Journal ID: ISSN 2475-9953
Publisher:
American Physical Society (APS)
Research Org:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Sponsoring Org:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Materials Sciences & Engineering Division
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; diffusion quantum Monte Carlo
OSTI Identifier:
1474475
Alternate Identifier(s):
OSTI ID: 1464575

Saritas, Kayahan, Krogel, Jaron T., Kent, P. R. C., and Reboredo, Fernando A.. Diffusion Monte Carlo: A pathway towards an accurate theoretical description of manganese oxides. United States: N. p., Web. doi:10.1103/PhysRevMaterials.2.085801.
Saritas, Kayahan, Krogel, Jaron T., Kent, P. R. C., & Reboredo, Fernando A.. Diffusion Monte Carlo: A pathway towards an accurate theoretical description of manganese oxides. United States. doi:10.1103/PhysRevMaterials.2.085801.
Saritas, Kayahan, Krogel, Jaron T., Kent, P. R. C., and Reboredo, Fernando A.. 2018. "Diffusion Monte Carlo: A pathway towards an accurate theoretical description of manganese oxides". United States. doi:10.1103/PhysRevMaterials.2.085801.
@article{osti_1474475,
title = {Diffusion Monte Carlo: A pathway towards an accurate theoretical description of manganese oxides},
author = {Saritas, Kayahan and Krogel, Jaron T. and Kent, P. R. C. and Reboredo, Fernando A.},
abstractNote = {Here, we present diffusion Monte Carlo (DMC) results for equation of state and quasiparticle gaps of manganese binary oxides MnO and MnO2 and the ternary oxide LaMnO3. Owing to the limited approximations made and the direct treatment of electronic correlations, our DMC-based study correctly describes structural properties such as the lattice constant, bulk moduli, and cohesive energies. It correctly predicts the ground-state phase of these oxides, which have different valences. Our study demonstrates the capability of DMC methods to predict the structural properties of highly correlated systems, which have been identified as suitable candidates for many applications ranging from catalysis to electronic devices. Our study also serves as a benchmark for both the manganese pseudopotential and other methodological choices to be used in calculations of similar oxides.},
doi = {10.1103/PhysRevMaterials.2.085801},
journal = {Physical Review Materials},
number = 8,
volume = 2,
place = {United States},
year = {2018},
month = {8}
}

Works referenced in this record:

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

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

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

Design principles for oxygen-reduction activity on perovskite oxide catalysts for fuel cells and metal–air batteries
journal, June 2011
  • Suntivich, Jin; Gasteiger, Hubert A.; Yabuuchi, Naoaki
  • Nature Chemistry, Vol. 3, Issue 7, p. 546-550
  • DOI: 10.1038/nchem.1069

Metal-insulator transitions
journal, October 1998
  • Imada, Masatoshi; Fujimori, Atsushi; Tokura, Yoshinori
  • Reviews of Modern Physics, Vol. 70, Issue 4, p. 1039-1263
  • DOI: 10.1103/RevModPhys.70.1039