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Title: Zirconia and hafnia polymorphs: Ground-state structural properties from diffusion Monte Carlo

Zirconia (zirconium dioxide) and hafnia (hafnium dioxide) are binary oxides used in a range of applications. Because zirconium and hafnium are chemically equivalent, they have three similar polymorphs, and it is important to understand the properties and energetics of these polymorphs. However, while density functional theory calculations can get the correct energetic ordering, the energy differences between polymorphs depend very much on the specific density functional theory approach, as do other quantities such as lattice constants and bulk modulus. We have used highly accurate quantum Monte Carlo simulations to model the three zirconia and hafnia polymorphs. We compare our results for structural parameters, bulk modulus, and cohesive energy with results obtained from density functional theory calculations. We also discuss comparisons of our results with existing experimental data, in particular for structural parameters where extrapolation to zero temperature can be attempted. We hope our results of structural parameters as well as for cohesive energy and bulk modulus can serve as benchmarks for density-functional theory based calculations and as a guidance for future experiments.
Authors:
 [1] ;  [1] ;  [1] ;  [2] ;  [3] ;  [4] ;  [5] ;  [6]
  1. Argonne National Lab. (ANL), Argonne, IL (United States)
  2. Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States)
  3. Argonne National Lab. (ANL), Lemont, IL (United States)
  4. Argonne National Lab. (ANL), Lemont, IL (United States); Imperial College, London (United Kingdom)
  5. Northwestern Univ., Evanston, IL (United States)
  6. Argonne National Lab. (ANL), Lemont, IL (United States); Northwestern Univ., Evanston, IL (United States)
Publication Date:
Grant/Contract Number:
AC02-06CH11357
Type:
Accepted Manuscript
Journal Name:
Physical Review Materials
Additional Journal Information:
Journal Volume: 2; Journal Issue: 7; Journal ID: ISSN 2475-9953
Publisher:
American Physical Society (APS)
Research Org:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE
OSTI Identifier:
1465776
Alternate Identifier(s):
OSTI ID: 1459744

Shin, Hyeondeok, Benali, Anouar, Luo, Ye, Crabb, Emily, Lopez-Bezanilla, Alejandro, Ratcliff, Laura E., Jokisaari, Andrea M., and Heinonen, Olle. Zirconia and hafnia polymorphs: Ground-state structural properties from diffusion Monte Carlo. United States: N. p., Web. doi:10.1103/PhysRevMaterials.2.075001.
Shin, Hyeondeok, Benali, Anouar, Luo, Ye, Crabb, Emily, Lopez-Bezanilla, Alejandro, Ratcliff, Laura E., Jokisaari, Andrea M., & Heinonen, Olle. Zirconia and hafnia polymorphs: Ground-state structural properties from diffusion Monte Carlo. United States. doi:10.1103/PhysRevMaterials.2.075001.
Shin, Hyeondeok, Benali, Anouar, Luo, Ye, Crabb, Emily, Lopez-Bezanilla, Alejandro, Ratcliff, Laura E., Jokisaari, Andrea M., and Heinonen, Olle. 2018. "Zirconia and hafnia polymorphs: Ground-state structural properties from diffusion Monte Carlo". United States. doi:10.1103/PhysRevMaterials.2.075001.
@article{osti_1465776,
title = {Zirconia and hafnia polymorphs: Ground-state structural properties from diffusion Monte Carlo},
author = {Shin, Hyeondeok and Benali, Anouar and Luo, Ye and Crabb, Emily and Lopez-Bezanilla, Alejandro and Ratcliff, Laura E. and Jokisaari, Andrea M. and Heinonen, Olle},
abstractNote = {Zirconia (zirconium dioxide) and hafnia (hafnium dioxide) are binary oxides used in a range of applications. Because zirconium and hafnium are chemically equivalent, they have three similar polymorphs, and it is important to understand the properties and energetics of these polymorphs. However, while density functional theory calculations can get the correct energetic ordering, the energy differences between polymorphs depend very much on the specific density functional theory approach, as do other quantities such as lattice constants and bulk modulus. We have used highly accurate quantum Monte Carlo simulations to model the three zirconia and hafnia polymorphs. We compare our results for structural parameters, bulk modulus, and cohesive energy with results obtained from density functional theory calculations. We also discuss comparisons of our results with existing experimental data, in particular for structural parameters where extrapolation to zero temperature can be attempted. We hope our results of structural parameters as well as for cohesive energy and bulk modulus can serve as benchmarks for density-functional theory based calculations and as a guidance for future experiments.},
doi = {10.1103/PhysRevMaterials.2.075001},
journal = {Physical Review Materials},
number = 7,
volume = 2,
place = {United States},
year = {2018},
month = {7}
}

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