mdh.sePublications
Change search
CiteExportLink to record
Permanent link

Direct link
Cite
Citation style
  • apa
  • ieee
  • modern-language-association-8th-edition
  • vancouver
  • Other style
More styles
Language
  • de-DE
  • en-GB
  • en-US
  • fi-FI
  • nn-NO
  • nn-NB
  • sv-SE
  • Other locale
More languages
Output format
  • html
  • text
  • asciidoc
  • rtf
Benchmarking Density Functional Theory Functionals for Polarons in Oxides: Properties of CeO2
Mälardalen University, School of Education, Culture and Communication. Nottingham Trent University, UK.ORCID iD: 0000-0001-6790-6569
Nottingham Trent University, UK.
Uppsala University, Sweden.ORCID iD: 0000-0003-3570-0050
2019 (English)In: The Journal of Physical Chemistry C, ISSN 1932-7447, E-ISSN 1932-7455, Vol. 123, no 9, p. 5164-5175Article in journal (Refereed) Published
Abstract [en]

We examine methods for studying polarons in metal oxides with density functional theory (DFT), using the example of cerium dioxide and the functionals, local density approximation + U (LDA+U), generalized gradient approximation + U (GGA+U) in the Perdew-Burke-Ernzerhof parametrization (PBE+U), as well as the hybrid functionals B3LYP, Heyd?Scuseria?Ernzerhof (HSE)03, HSE06, and PBE0. We contrast the four polaron energies commonly reported in different parts of the literature: formation energy, localization/relaxation energy, density-of-states level, and polaron-hopping activation barrier. Qualitatively, all these functionals predict "small" (Holstein) polarons on the scale of a single lattice site, although LDA+U and GGA+U are more effective than the hybrids at localizing the Ce 4f electrons. The improvements over pure LDA/GGA appear because of changes in the filled Ce 4f states when using LDA/GGA+U but due to changes in the empty Ce 4f states when using the hybrids. DFT is shown to have sufficient correlation to predict both adiabatic and (approximate) diabatic hopping barriers. Overall, LDA+U = 6 eV provides the best description in comparison to the experiment, followed by GGA+U = 5 eV. The hybrids are worse, tending to overestimate the gap and significantly underestimate the polaron-hopping barriers.

Place, publisher, year, edition, pages
American Chemical Society , 2019. Vol. 123, no 9, p. 5164-5175
Keywords [en]
Density Functional Theory, Ceria, Oxides, Polarons
National Category
Physical Sciences
Identifiers
URN: urn:nbn:se:mdh:diva-42942DOI: 10.1021/acs.jpcc.8b09134ISI: 000460996000002Scopus ID: 2-s2.0-85062622244OAI: oai:DiVA.org:mdh-42942DiVA, id: diva2:1298286
Available from: 2019-03-22 Created: 2019-03-22 Last updated: 2019-05-15Bibliographically approved

Open Access in DiVA

The full text will be freely available from 2020-01-24 15:26
Available from 2020-01-24 15:26

Other links

Publisher's full textScopus

Authority records BETA

Castleton, Christopher

Search in DiVA

By author/editor
Castleton, ChristopherKullgren, J.
By organisation
School of Education, Culture and Communication
In the same journal
The Journal of Physical Chemistry C
Physical Sciences

Search outside of DiVA

GoogleGoogle Scholar

doi
urn-nbn

Altmetric score

doi
urn-nbn
Total: 21 hits
CiteExportLink to record
Permanent link

Direct link
Cite
Citation style
  • apa
  • ieee
  • modern-language-association-8th-edition
  • vancouver
  • Other style
More styles
Language
  • de-DE
  • en-GB
  • en-US
  • fi-FI
  • nn-NO
  • nn-NB
  • sv-SE
  • Other locale
More languages
Output format
  • html
  • text
  • asciidoc
  • rtf