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Performance of DFT+ U method for prediction of structural and thermodynamic parameters of monazite‐type ceramics
Author(s) -
Blanca Romero Ariadna,
Kowalski Piotr M.,
Beridze George,
Schlenz Hartmut,
Bosbach Dirk
Publication year - 2014
Publication title -
journal of computational chemistry
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 0.907
H-Index - 188
eISSN - 1096-987X
pISSN - 0192-8651
DOI - 10.1002/jcc.23618
Subject(s) - density functional theory , ab initio , hubbard model , monazite , thermodynamics , type (biology) , materials science , computational chemistry , chemistry , physics , condensed matter physics , quantum mechanics , superconductivity , nuclear physics , zircon , ecology , biology
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. © 2014 Wiley Periodicals, Inc.