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Temperature dependence of (111) and (110) ceria surface energy
KTH Royal Inst Technol, Brinellvagen 23, S-10044 Stockholm, Sweden..
Univ Stuttgart, Inst Mat Sci, D-70569 Stuttgart, Germany..
KTH Royal Inst Technol, Brinellvagen 23, S-10044 Stockholm, Sweden.;Mat Ctr Leoben Forsch GmbH, Roseggerstr 12, A-8700 Leoben, Austria..
Uppsala University, Disciplinary Domain of Science and Technology, Physics, Department of Physics and Astronomy, Materials Theory. KTH Royal Inst Technol, Brinellvagen 23, S-10044 Stockholm, Sweden.
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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, 2023. Vol. 107, no 3, article id 035407
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Condensed Matter Physics
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URN: urn:nbn:se:uu:diva-500326DOI: 10.1103/PhysRevB.107.035407ISI: 000956927600002OAI: oai:DiVA.org:uu-500326DiVA, id: diva2:1750957
Funder
Swedish National Infrastructure for Computing (SNIC), SNIC 2021/3-36Swedish National Infrastructure for Computing (SNIC), SNIC 2022/1-30Swedish National Infrastructure for Computing (SNIC), SNIC 2022/22-106Swedish Research CouncilCarl Tryggers foundation , CTS 20-206EU, Horizon 2020, 865855Available from: 2023-04-14 Created: 2023-04-14 Last updated: 2023-04-14Bibliographically approved

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Johansson, Börje

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