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Temperature dependence of (111) and (110) ceria surface energy
KTH, School of Industrial Engineering and Management (ITM), Materials Science and Engineering.
Univ Stuttgart, Inst Mat Sci, D-70569 Stuttgart, Germany..
KTH, School of Industrial Engineering and Management (ITM), Materials Science and Engineering, Structures. Mat Ctr Leoben Forsch GmbH, Roseggerstr 12, A-8700 Leoben, Austria..ORCID iD: 0000-0002-3880-0965
KTH, School of Industrial Engineering and Management (ITM), Materials Science and Engineering. Uppsala Univ, Dept Phys & Astron, Div Mat Theory, S-75120 Uppsala, Sweden..ORCID iD: 0000-0001-5429-5578
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2023 (English)In: Physical Review B, ISSN 2469-9950, E-ISSN 2469-9969, Vol. 107, no 3, article id 035407Article in journal (Refereed) Published
Abstract [en]

High-temperature properties of ceria surfaces are important for many applications. Here, we report the temperature dependencies of surface energy for (111) and (110) CeO2 obtained in the framework of the extended two-stage up-sampled thermodynamic integration using Langevin dynamics. The method was used together with machine-learning potentials called moment tensor potentials (MTPs), which were fitted to the results of the ab initio molecular dynamics calculations for (111) and (110) CeO2 at different temperatures. The parameters of MTP training and fitting were tested, and the optimal algorithm for the ceria systems was proposed. We found that the temperature increases from 0 to 2100 K led to the decrease of the Helmholtz free energy of (111) CeO2 from 0.78 to 0.64 J/m2. The energy of (110) CeO2 dropped from 1.19 J/m2 at 0 K to 0.92 J/m2 at 1800 K. We show that it is important to consider anharmonicity, as simple consideration of volume expansion gives the wrong temperature dependencies of the surface energies.

Place, publisher, year, edition, pages
American Physical Society (APS) , 2023. Vol. 107, no 3, article id 035407
National Category
Inorganic Chemistry
Identifiers
URN: urn:nbn:se:kth:diva-326054DOI: 10.1103/PhysRevB.107.035407ISI: 000956927600002Scopus ID: 2-s2.0-85146311930OAI: oai:DiVA.org:kth-326054DiVA, id: diva2:1752865
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QC 20230425

Available from: 2023-04-25 Created: 2023-04-25 Last updated: 2023-04-25Bibliographically approved

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Kholtobina, Anastasiia S.Ruban, Andrei V.Johansson, BörjeSkorodumova, Natalia

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Physical Review B
Inorganic Chemistry

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