Performance of DFT+U method for prediction of structural and thermodynamic parameters of monazite-type ceramics.
We performed a density functional theory (DFT) study of the monazite-type ceramics using DFT+U method, where the Hubbard U parameters are derived ab initio, with the main goal in testing the predictive power of this computational method for modeling of f-electron materials that are of interest in nuclear waste management. We show that DFT+U approach with PBEsol as the exchange-correlation functional significantly improves description of structures and thermodynamic parameters of lanthanide-bearing oxides and monazites over commonly used standard DFT (PBE) approach. We found that it is essential to use the Hubbard U parameter derived for a given element and a given structure to reproduce the structural parameters of the measured materials. We obtained exceptionally good description of the structural parameters with U parameter derived using the linear response approach of Cococcioni and de Gironcoli (Phys. Rev. B 2005, 71, 035105). This shows that affordable methods, such as DFT+U with a clever choice of exchange-correlation functional and the Hubbard U parameter can lead to a good description of f-electron materials.
Institute of Energy and Climate Research, Nuclear Waste Management and Reactor Safety, Forschungszentrum Jülich, Wilhelm-Johnen-Strasse, 52428, Jülich, Germany; JARA High-Performance Computing, Schinkelstrasse 2, 52062, Aachen, Germany.
Ariadna
A
Blanca Romero
Piotr M
PM
Kowalski
George
G
Beridze
Hartmut
H
Schlenz
Dirk
D
Bosbach
ab initio calculations; computational chemistry; density functional calculations; lanthanides; solid-state reactions