Zirconia and hafnia polymorphs: Ground-state structural properties from diffusion Monte Carlo
File(s)MG10041_accepted.pdf (3.92 MB)
Accepted version
Author(s)
Type
Journal Article
Abstract
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.
Date Issued
2018-07-11
Date Acceptance
2018-06-26
Citation
Physical Review Materials, 2018, 2 (7)
ISSN
2475-9953
Publisher
American Physical Society
Journal / Book Title
Physical Review Materials
Volume
2
Issue
7
Copyright Statement
©2018 American Physical Society
Identifier
http://gateway.webofknowledge.com/gateway/Gateway.cgi?GWVersion=2&SrcApp=PARTNER_APP&SrcAuth=LinksAMR&KeyUT=WOS:000438196300004&DestLinkType=FullRecord&DestApp=ALL_WOS&UsrCustomerID=1ba7043ffcc86c417c072aa74d649202
Subjects
Science & Technology
Technology
Materials Science, Multidisciplinary
Materials Science
OXIDE THIN-FILMS
ELECTRICAL CHARACTERISTICS
NANOCRYSTALLINE ZIRCONIA
PHASE-TRANSFORMATION
RELATIVE STABILITY
OPTICAL-PROPERTIES
THERMAL-EXPANSION
CRYSTAL-STRUCTURE
ZRO2 POLYMORPHS
HFO2
Publication Status
Published
Article Number
ARTN 075001