Modeling of CeO2, Ce2O3, and CeO2-x in the LDA plus U formalism
2007 (English)In: Physical Review B. Condensed Matter and Materials Physics, ISSN 1098-0121, E-ISSN 1550-235X, 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.
IdentifiersURN: urn:nbn:se:uu:diva-146032DOI: 10.1103/PhysRevB.75.035109ISI: 000243895400042OAI: oai:DiVA.org:uu-146032DiVA: diva2:397417