Modeling of Ce2, Ce2O3 ,and CeO2-x in the LDA+U formalism
2007 (English)In: Physical Review B Condensed Matter, ISSN 0163-1829, E-ISSN 1095-3795, Vol. 75, no 3, 035109- p.Article in journal (Refereed) Published
The electronic structure and thermodynamic properties of CeO2 and Ce2O3 have been studied from first principles by the all-electron projector-augmented-wave (PAW) method, as implemented in the ab initio total-energy and molecular-dynamics program VASP (Vienna ab initio simulation package). The local density approximation (LDA)+U formalism has been used to account for the strong on-site Coulomb repulsion among the localized Ce 4f electrons. We discuss how the properties of CeO2 and Ce2O3 are affected by the choice of U as well as the choice of exchange-correlation potential, i.e., the local density approximation or the generalized gradient approximation. Further, reduction of CeO2, leading to formation of Ce2O3 and CeO2-x, and its dependence on U and exchange-correlation potential have been studied in detail. Our results show that by choosing an appropriate U it is possible to consistently describe structural, thermodynamic, and electronic properties of CeO2, Ce2O3, and CeO2-x, which enables modeling of redox processes involving ceria-based materials.
Place, publisher, year, edition, pages
2007. Vol. 75, no 3, 035109- p.
Other Engineering and Technologies not elsewhere specified
IdentifiersURN: urn:nbn:se:kth:diva-6888DOI: 10.1103/PhysRevB.75.035109ISI: 000243895400042ScopusID: 2-s2.0-33846442083OAI: oai:DiVA.org:kth-6888DiVA: diva2:11728
QC 201006222007-03-142007-03-142012-03-22Bibliographically approved